Country：Japan

Language：English   Publishing type：Research paper (scientific journal)   Publisher：ACS Applied Nano Materials  

The in-plane orientation of the nanowalls was successfully realized through control of the ion energy and incidence angle during plasma-enhanced chemical vapor deposition processing of carbon nanowalls (CNWs). The ion energy and incidence angle were controlled by using a tilted stage, a metal mesh, and a radiofrequency (RF) stage bias. The degree of in-plane orientation was strongly dependent on the ion energy and incidence angle. The maximum degree of in-plane orientation was 0.65 for a stage tilt angle of 75° and an RF bias of 6 W. In the in-plane X-ray diffraction pattern, a graphite 002 peak was observed at a diffraction angle of 25.7° only when the X-rays were incident along the in-plane orientation direction of the CNWs. The electrical conductivity of the in-plane oriented CNWs was measured using the four-point probe method, and the in-plane conductivity was determined to be 2.5 times larger than that in the perpendicular direction. The conductivity was also improved by a factor of 2 compared to random CNWs. These results show that control of the degree of in-plane orientation leads to anisotropic electrical properties for vertically grown nanographene.

DOI： 10.1021/acsanm.4c01771

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Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Applied Surface Science  

A novel concept and process were proposed for the plasma-enhanced atomic layer deposition (PE-ALD) of carbon films. α, α’-dichloro-p-xylene (DCX) was used to form the adsorption layer, which was modified using nitrogen/hydrogen (N2/H2) plasma. Through iterative molecular chemisorption and end-group substitution processes, the selective and precise control of carbon deposition by PE-ALD was achieved. The growth per cycle of this process was estimated to be 0.02–0.05 nm/cycle. To determine the chemical reactions that occurred during the PE-ALD process, the IR spectra observed using in-situ Fourier transform infrared spectroscopy were analyzed. The decrease in the Si-OH bond at 3740 cm−1 and the saturation of the increase in CH bending at 1250 cm−1 revealed that the deposition of a DCX monolayer via a dehydrochlorination reaction with isolated OH bonding on SiO2 has been successfully achieved. The change in N(−H)x stretching during the N2/H2 plasma treatment indicated the substitution of exposed C-Cl bonding with C-NH2 bonding on the chemisorbed DCX monolayer surface. Additionally, the composition of the carbon films after 200-cycle PE-ALD was analyzed. Finally, the realization of the concept for PE-ALD of carbon film was confirmed by surface analysis.

DOI： 10.1016/j.apsusc.2024.161485

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Diamond and Related Materials  

The synergetic effects of process parameters on hydrogenated amorphous carbon (a-C:H) films properties were quantitatively analyzed in plasma-enhanced chemical vapor deposition. Predictive models, created from experimental datasets and machine learning, indicate a synergetic effect between the H2 ratio and ion energy impacting on the substrate. At a H2 ratio of 75 %, etch rates of 200 nm/min were predicted, regardless of radio frequency (RF) bias. These rates decreased to 120–140 nm/min at lower H2 ratios, primarily depending on RF bias. Quadrupole mass spectrometry and Raman scattering were used to investigate the underlying mechanisms. High H2 ratios led to a greater presence of low-mass hydrogen-rich molecules in the plasma. The C2H3 radical intensity at a 75 % H2 ratio was 15 times greater than that at 0 % at an RF bias of 50 W, and similar trends were observed for other low-mass neutrals. The synergetic effects of H2 ratio and RF bias decreased the film's hydrogen content. Machine learning and those diagnostics revealed that ion bombardment induces dehydrogenation of a-C:H, influenced by hydrogen-rich species. This study demonstrates that machine learning can uncover complex plasma processes and optimize material synthesis.

DOI： 10.1016/j.diamond.2024.111687

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Scientific Reports  

Correction to: Scientific Reportshttps://doi.org/10.1038/s41598-024-61501-9, published online 13 May 2024 The original version of this Article contained an error in the legend of Figures 20 and 21, where an inset was mistakenly included. Figure 20 “GaN on a GaN template under the best conditions with a growth time of 15 min. (a) Surface morphology (inset is the RHEED pattern), (b) cross-section by SEM and (c) the omega scan of thin and thick GaN. Growth conditions; 800 °C, 600 W, 300 Pa, TMG + 5 °C/H2 carrier gas 20 sccm.” now reads, “GaN on a GaN template under the best conditions with a growth time of 15 min. (a) Surface morphology, (b) cross-section by SEM and (c) the omega scan of thin and thick GaN. Growth conditions; 800 °C, 600 W, 300 Pa, TMG + 5 °C/H2 carrier gas 20 sccm.” And Figure 21 “GaN on a bulk GaN substrate under the best conditions with a growth time of 15 min. (a) Surface morphology (inset is the RHEED pattern), (b) cross-section by SEM and (c) the omega scan of thin and thick GaN. Growth conditions; 800 °C, 600 W, 300 Pa, TMG + 5 °C/H2 carrier gas 20 sccm.” now reads, “GaN on a bulk GaN substrate under the best conditions with a growth time of 15 min. (a) Surface morphology, (b) cross-section by SEM and (c) the omega scan of thin and thick GaN. Growth conditions; 800 °C, 600 W, 300 Pa, TMG + 5 °C/H2 carrier gas 20 sccm.” The original Article has been corrected.

DOI： 10.1038/s41598-024-82619-w

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PubMed

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Small Methods  

Manufacturing semiconductor devices requires advanced patterning technologies, including reactive ion etching (RIE) based on the synergistic interactions between ions and etch gas. However, these interactions weaken as devices continuously scale down to sub-nanoscale, primarily attributed to the diminished transport of radicals and ions into the small features. This leads to a significant decrease in etch rate (ER). Here, a novel synergistic interaction involving ions, surface-adsorbed chemistries, and materials at cryogenic temperatures is found to exhibit a significant increase in the ER of SiO2 using CF4/H2 plasmas. The ER increases twofold when plasma with H2/(CF4 + H2) = 33% is used and the substrate temperature is lowered from 20 to −60 °C. The adsorption of HF and H2O on the SiO2 surface at cryogenic temperatures is confirmed using in situ Fourier transform infrared spectroscopy. The synergistic interactions of the surface-adsorbed HF/H2O as etching catalysts and plasma species result in the ER enhancement. Therefore, a mechanism called “pseudo-wet plasma etching” is proposed to explain the cryogenic etching process. This synergy demonstrates that the enhanced etch process is determined by the surface interactions between ions, surface-adsorbed chemistry, and the material being etched, rather than interactions between ion and gas phase, as observed in the conventional RIE.

DOI： 10.1002/smtd.202400090

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PubMed

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Free Radical Research  

DOI： 10.1080/10715762.2023.2297343

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PubMed

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Applied Surface Science  

Graphene sheet transferred onto the SiO2 substrate has various types at different regions such as single-layer graphene (SLG), double-layer graphene (DLG), and multi-layer graphene (MLG). These layers were identified by Raman analysis of 2D band position around 2700 cm−1 and full width at half maximum (FWHM). The transferred graphene sheets on SiO2 were remotely irradiated by oxygen plasma without energetic ions at a room temperature. At the beginning of the oxygen plasma irradiation, the carbons on the surface of the graphene sheets were oxidized and the 2D-FWHMs were broadened due to an increase of defects on the basal plane. By controlling the plasma irradiation time up to 120 min, selectively stripping away the SLG regions on the SiO2 surface was observed while leaving the other DLG and MLG regions. The difference in attractive forces resulted in favorable desorption of carbon atoms occurred in the oxidized SLG regions on SiO2 surface by the remote oxygen plasma irradiation.

DOI： 10.1016/j.apsusc.2024.160598

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Coatings  

Heel marks (HMs) are a type of dirt stain consisting of polyester-based urethane rubber on polyvinyl chloride (PVC) floor surfaces. The rapid removal of HMs was achieved by using non-thermal atmospheric-pressure plasma technology. Mimetic HMs were prepared by coating PVC floor samples with HMs to a thickness of 13.9 μm. The removal area, thickness, and volume were measured after applying spark discharges at high voltage and a repetition rate of 50 kHz. The treated surfaces were analyzed by using X-ray photoelectron spectroscopy (XPS) and pyrolysis–gas chromatography with time-of-flight mass spectrometry (Py-GC/TOFMS). Removal rates of 20 mm2/min in area, 52 mm3/min in volume, and 7 μm/min in depth were achieved with an inter-electrode distance of 10.0 mm and an air flow rate of 20 standard liters per minute. A removal depth of 10 μm/min was achieved without air supply. The mechanism of stain removal by spark discharge was modeled by decomposing the original high-molecular-weight molecules in polyester-based urethane rubber into low-molecular-weight molecules, such as methylene diisocyanate (MDI) components. The results of this study may facilitate the development of a novel electric vacuum cleaner capable of removing floor stains.

DOI： 10.3390/coatings14101339

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Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：ACS Applied Materials and Interfaces  

Ternary metal carbide TiAlC has been proposed as a metal gate material in logic semiconductor devices. It is a hard-to-etch material due to the low volatility of the etch byproducts. Here, a simple, highly controllable, and dry etching method for TiAlC has been first presented using nonhalogen N2/H2 plasmas at low pressure (several Pa) and 20 °C. A capacitively coupled plasma etcher was used to generate N2/H2 plasmas containing active species, such as N, NH, and H to modify the metal carbide surface. The etch rate of TiAlC was obtained at 3 nm/min by using the N2/H2 plasma, whereas no etching occurred with pure N2 plasma or pure H2 plasma under the same conditions. The surface roughness of the TiAlC film etched by N2/H2 plasma was controlled at the atomic level. A smooth etched surface was achieved with a root-mean-square roughness of 0.40 nm, comparable to the initial roughness of 0.44 nm. The plasma properties of the N2/H2 plasmas were diagnosed by using a high-resolution optical emission spectrometer, detecting the NH molecular line at 336 nm. The etching behavior and plasma-surface reaction between N2/H2 plasma and TiAlC were investigated by using in situ spectroscopic ellipsometry, in situ attenuated total reflectance-Fourier transform infrared spectrometry, and X-ray photoelectron spectroscopy. The findings indicate that the N-H, C-N, and Ti(Al)-N bonds form on the TiAlC surface etched by the N2/H2 plasmas. The mechanism for etching of TiAlC involving transformation reactions between inorganic materials (metal carbides) and inorganic etchants (N2/H2 plasma) to form volatile organic compounds such as methylated, methyl-aminated, and aminated metals is proposed. Nonhalogen or nonorganic compound etchants were used during the etching process. The study provides useful insights into microfabrication for large-scale integrated circuits.

DOI： 10.1021/acsami.4c11025

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PubMed

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Japanese Journal of Applied Physics, Part 1: Regular Papers and Short Notes and Review Papers  

DOI： 10.35848/1347-4065/ad5d78

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Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Advanced Engineering Materials  

Recent advances in the growth of carbon nanowalls (CNWs) and vertical graphene nanosheets using various plasma-enhanced chemical vapor deposition (PECVD) methods are reviewed in this article. Growth methods are classified into hot- and cold-wall reactors equipped with diverse plasma generation systems, and their respective characteristics are summarized, with particular attention to the behavior of reactive species, such as ions and radicals, generated within the plasma. Recent progress in this research domain is outlined for each method, and an organized account of the chemical kinetic phenomena occurring within the plasma is provided. Finally, future perspectives are discussed. Fundamental data are obtained through real-time in situ measurements of ions and radicals, and the construction of a database from these data offers microscopic insights that significantly enhance processing outcomes for macroscopically controlling the mechanical shapes and chemical properties of CNWs.

DOI： 10.1002/adem.202400679

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Faraday Discussions  

Plasma-activated Ringer's lactate solutions (PALs), which are Ringer's lactate solutions treated with non-thermal atmospheric-pressure plasma, have an anti-tumor effect and can be used for chemotherapy. As the anti-tumor effect of the PAL is influenced by the cell-treatment time, it is necessary to monitor the structural changes of the cell surface with non-invasive, nanoscale, and time-lapse imaging to understand the anti-tumor effect. In this study, to characterize the anti-tumor effect of the PAL, we used scanning ion conductance microscopy (SICM), using glass nanopipettes as probes, to visualize the structural changes of the cell surface. SICM time-lapse topographic imaging visualized a decrease in the movement of lamellipodia in normal cells and cancer cells after the PAL treatment. Furthermore, in normal cells, protrusive structures were observed on the cell surface. Time-lapse imaging using SICM allowed us to characterize the differences in the morphological changes between the normal and cancer cells upon exposure to the PAL.

DOI： 10.1039/d4fd00116h

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PubMed

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Journal of Vacuum Science and Technology B  

Plasma etching is an essential semiconductor manufacturing technology required to enable the current microelectronics industry. Along with lithographic patterning, thin-film formation methods, and others, plasma etching has dynamically evolved to meet the exponentially growing demands of the microelectronics industry that enables modern society. At this time, plasma etching faces a period of unprecedented changes owing to numerous factors, including aggressive transition to three-dimensional (3D) device architectures, process precision approaching atomic-scale critical dimensions, introduction of new materials, fundamental silicon device limits, and parallel evolution of post-CMOS approaches. The vast growth of the microelectronics industry has emphasized its role in addressing major societal challenges, including questions on the sustainability of the associated energy use, semiconductor manufacturing related emissions of greenhouse gases, and others. The goal of this article is to help both define the challenges for plasma etching and point out effective plasma etching technology options that may play essential roles in defining microelectronics manufacturing in the future. The challenges are accompanied by significant new opportunities, including integrating experiments with various computational approaches such as machine learning/artificial intelligence and progress in computational approaches, including the realization of digital twins of physical etch chambers through hybrid/coupled models. These prospects can enable innovative solutions to problems that were not available during the past 50 years of plasma etch development in the microelectronics industry. To elaborate on these perspectives, the present article brings together the views of various experts on the different topics that will shape plasma etching for microelectronics manufacturing of the future.

DOI： 10.1116/6.0003579

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Vacuum  

The synthesis of carbon nanowalls (CNWs) necessitated a substrate heating temperature above 600 °C. This study describes a low-temperature growth at 225 °C and characterization of CNWs synthesized by the radical injection plasma-enhanced chemical vapor deposition. To investigate the effect of temperature on the growth process, CNWs were synthesized at various temperatures ranging from 200 °C to 700 °C. The morphology of the CNWs observed with a scanning electron microscope shows that wall density increases as substrate temperature decreases. The Raman spectroscopy analysis indicates that CNWs grown at 225 °C have higher defect levels than those grown at higher temperatures, such as 700 °C. Transmission electron microscopy confirmed the presence of multiple graphene layers in the CNWs grown at 225 °C. The water contact angle results revealed that CNWs grown at 225 °C had higher hydrophobicity than those grown at higher temperatures, opening up the potential for CNW applications.

DOI： 10.1016/j.vacuum.2024.113180

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CiNii Research

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Scientific Reports  

Using our recently developed radical-enhanced metalorganic chemical vapor deposition (REMOCVD) technique, we have grown gallium nitride (GaN) on bulk GaN and GaN on Si templates. Three features make up this system: (1) applying very high-frequency power (60 MHz) to increase the plasma density; (2) introducing H2 and N2 gas in the plasma discharge region to produce active NHx radical species in addition to nitrogen radicals; and (3) supplying radicals under remote plasma arrangement with a Faraday cage to suppress charged ions and photons. Using this new REMOCVD system, it was found that high-quality crystals can be grown at lower temperatures than that of MOCVD but the disadvantage was that the growth rate was smaller as 0.2–0.8 μm/h than that by MOCVD. In the present work, we have used a pBN inner shield to prevent the deactivation of radicals to increase the growth rate. The growth conditions such as the plasma power, trimethylgallium (TMG) source flow rate, N2 + H2 gas mixture flow rate, and the ratio of N2/H2 were optimized and it was found that the growth rate could be increased up to 3.4 μm/h with remarkably high crystalline quality comparable to that of MOCVD. The XRD-FWHM of GaN grown on the GaN/Si template and the bulk GaN substrate were 977 arcsec and 72 arcsec respectively. This work may be very promising to achieve high-power GaN/GaN devices.

DOI： 10.1038/s41598-024-61501-9

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PubMed

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Journal of Vacuum Science and Technology A: Vacuum, Surfaces and Films  

Ar ions with controlled energy and doses, along with radicals in CF4 plasma, were irradiated separately onto a Si (111) 7 × 7 surface by using a plasma beam reactor. The crystal structure and the chemical bonds on the surface were analyzed by scanning tunneling microscopy, atomic force microscopy, and x-ray photoelectron spectroscopy without air exposure of the samples. The SiF layer formed by F radical irradiation was completely removed by a desorption reaction induced by heating at 600 °C, resulting in an atomically flat surface that maintained the crystal structure. The 7 × 7 structure, which was reconstructed by each irradiation process alone, was not reconstructed because of the synergistic effects of F radicals and Ar ions in the cyclic CF4/Ar plasma used to simulate an atomic layer etching process. The cyclic CF4/Ar plasma process inhibited the reconstruction of the crystal structure by forming a mixture region that included Si, F, and C atoms.

DOI： 10.1116/6.0003432

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Thin Solid Films  

The plasma functionalization of carbon nanowalls (CNWs) is of great interest due to their potential applications in electron field emission and energy storage devices. In this study, the effects of nitrogen on the growth and properties of CNWs are thoroughly investigated by varying a wide range of the N2 concentrations in the CH4/H2/N2 discharge plasma. Nitrogen-doped carbon nanowalls (N–CNWs) were synthesized in a single-step growth using the hydrogen radical injection plasma-enhanced chemical vapor deposition technique. The formation of dense N–CNWs was found to be enhanced by nitrogen and was three times higher in the sample with a 150 sccm N2 flow rate than in the sample without N2 addition (N-0). As the N2 concentration increased from 0 to 200 sccm, the morphology of CNWs changed from relatively straight to curly-like nanowall structures. A high-resolution optical emission spectroscopic observation shows that as N2 flow increased, CN radicals became the dominant species, suppressing the formation of C2 and CH. Photoelectron spectroscopy analysis revealed the nitrogen doping effect on graphene layers at high N2 concentrations. According to Raman and Transmission Electron Microscopy analyses, the N–CNWs had more branched and thicker nanowalls with higher defect concentrations than the N-0 sample. The wettability of N–CNWs was improved, particularly for the sample with a N2 flow rate of 150 sccm.

DOI： 10.1016/j.tsf.2024.140322

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CiNii Research

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Japanese Journal of Applied Physics  

The electronic properties of C4F6 were investigated by using computational chemistry to clarify the dissociative channels in the process plasma. The results show the mainly ionized ion is C3F3+ (CF2=C=CF+; propargyl ion) which is observed in the mass spectrum with the electron energy of 70 eV, and the intermediate molecular structure to produce C3F3+ ion is methyl allene ion (CF2=C=CF-CF3+). The molecular ion C4F6+ is also mainly produced in the ionization threshold region. For the excited states, the calculated results suggest that CF2CFCF + CF2 dissociation takes place in the energy region higher than 7.0 eV and C2F3 + C2F3 dissociation takes place in the energy region higher than 8.0 eV. In the electron attachment process, the vertical electron attachment energy was calculated as 1.1 eV and the nonadiabatic negative ion energy was −0.2 eV lower than the energy of neutral C4F6

DOI： 10.35848/1347-4065/ad3166

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CiNii Research

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Free Radical Research  

Non-thermal atmospheric pressure plasma (NTP), an ionized gas containing electrons, ions, radicals, and photons, has various biological effects, including wound healing and anticancer effects. Plasma-activated medium (PAM), which is prepared by irradiating medium with NTP, preferentially kills cancer cells. Large amounts of reactive oxygen species (ROS) and reactive nitrogen species (RNS) included in PAM are closely related to its anticancer effects. The precise mechanism of PAM-induced cytotoxicity is not fully understood; however, PAM exposure has been reported to reduce cellular energy metabolism. Glutamine (Gln) is an important amino acid as an energy source in cancer cells. Gln is converted to glutamate by glutaminase (GLS), and is utilized to synthesize ATP and glutathione (GSH). Expression levels of GLS have been shown to be higher in certain types of cancers. In this study, we examined the effects of GLS inhibition on PAM cytotoxicity using breast cancer MDA-MB-231 cells. Pretreatment with BPTES, a glutaminase 1 (GLS1) inhibitor, dose-dependently enhanced PAM-induced cell death. PAM-induced ROS production and γ-H2AX formation, a DNA damage marker, were increased in cells pretreated with BPTES compared with PAM alone. BPTES pretreatment enhanced a PAM-induced decrease in intracellular GSH, indicating the possibility that BPTES reduces the antioxidant capacity of MDA-MB-231 cells. In addition, BPTES pretreatment enhanced PAM-induced loss of the mitochondrial membrane potential and reduction of ATP production. Moreover, GLS1 knockdown promoted PAM-induced cell death. Taken together, the combination of GLS1 inhibitors such as BPTES is considered to be useful for enhancing the cytotoxic effects of PAM against cancer cells.

DOI： 10.1080/10715762.2024.2332343

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CiNii Research

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Plasma  

Plasma-driven science is defined as the artificial control of physical plasma-driven phenomena based on complex interactions between nonequilibrium open systems. Recently, peculiar phenomena related to physical plasma have been discovered in plasma boundary regions, either naturally or artificially. Because laboratory plasma can be produced under nominal conditions around atmospheric pressure and room temperature, phenomena related to the interaction of plasma with liquid solutions and living organisms at the plasma boundaries are emerging. Currently, the relationships between these complex interactions should be solved using science-based data-driven approaches; these approaches require a reliable and comprehensive database of dynamic changes in the chemical networks of elementary reactions. Consequently, the elucidation of the mechanisms governing plasma-driven phenomena and the discovery of the latent actions behind these plasma-driven phenomena will be realized through plasma-driven science.

DOI： 10.3390/plasma7010011

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CiNii Research

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Free Radical Biology and Medicine  

Reactive species are involved in various aspects of neoplastic diseases, including carcinogenesis, cancer-specific metabolism and therapeutics. Non-thermal plasma (NTP) can directly provide reactive species, by integrating atmospheric and interjacent molecules as substrates, to represent a handy strategy to load oxidative stress in situ. NTP causes apoptosis and/or ferroptosis specifically in cancer cells of various types. Plasma-activated Ringer's lactate (PAL) is another modality at the preclinical stage as cancer therapeutics, based on more stable reactive species. PAL specifically kills malignant mesothelioma (MM) cells, employing lysosomal ·NO as a switch from autophagy to ferroptosis. However, the entire molecular mechanisms have not been elucidated yet. Here we studied cytosolic iron regulations in MM and other cancer cells in response to PAL exposure. We discovered that cells with higher catalytic Fe(II) are more susceptible to PAL-induced ferroptosis. PAL caused a cytosolic catalytic Fe(II)-associated pathology through iron chaperones, poly (rC)-binding proteins (PCBP)1/2, inducing a disturbance in glutathione-regulated iron homeostasis. PCBP1/NCOA4-mediated ferritinophagy started at a later phase, further increasing cytosolic catalytic Fe(II), ending in ferroptosis. In contrast, PCBP2 after PAL exposure contributed to iron loading to mitochondria, leading to mitochondrial dysfunction. Therapeutic effect of PAL was successfully applied to an orthotopic MM xenograft model in mice. In conclusion, PAL can selectively sensitize MM cells to ferroptosis by remodeling cytoplasmic iron homeostasis, where glutathione and PCBPs play distinct roles, resulting in lethal ferritinophagy and mitochondrial dysfunction. Our findings indicate the clinical application of PAL as a ferroptosis-inducer and the potential of PCBPs as novel targets in cancer therapeutics.

DOI： 10.1016/j.freeradbiomed.2024.02.001

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CiNii Research

Language：Japanese   Publishing type：Research paper (scientific journal)   Publisher：The Japan Society of Vacuum and Surface Science  

<p>A novel synthesis method of nanographene materials by using in-liquid plasma has been developed. By this method, the high synthesis rate of nanographene up to 1 mg/min. can be realized. There is a trade-off relationship between synthesis rate and crystallographic domain size with respect to the number of carbon atoms in the raw alcohol molecules. For example, when using 1-butanol (C₄H₉OH), the synthesis rate is approximately twice as high as when using ethanol (C₂H₅OH), but the domain size, which indicates crystallographic quality, is about half smaller. On the other hand, when using hexane (C₆H₁₄) or benzene (C₆H₆), the synthesis rate is approximately 17 times and 1.7 times faster than when using hexanol (C₆H₁₃OH), respectively, but their domain size is much smaller compared with that by ethanol. This indicates an effect of OH radicals on the domain size improvement. By adding iron (II) phthalocyanine, <i>etc.</i> to the alcohol raw material, nitrogen-doped nanographene materials were successfully synthesized and confirmed their catalytic activity. The mechanism of expression of catalytic activity was also clarified.</p>

DOI： 10.1380/vss.67.77

CiNii Research

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Applied Surface Science  

Etching of oxygen-based plasmas with sulfur dioxide (SO2) or carbonyl sulfide (OCS) can form high-aspect-ratio (HAR) features of amorphous carbon films as carbon hard masks (CHM). The etched profiles showing shapes such as bowing or tapering are essentially dependent on the partial pressures of SO2 or OCS in the O2 plasma. The surface treated after the OCS-added plasma exhibited strong sulfurization by S2 and CS species in S 2p of the X-ray photoelectron spectroscopy (XPS). The gas-phase interactions in the sulfur-oxygen-carbon system generated atoms and molecules, such as O, O+, and O2+, which etched at the bottom and, conversely, SO, CO, CS, CS2, and S2, which inhibited isotropic etching at the sidewalls of the HAR features. The chemical reactions of the CS sulfurizing precursors in the gas phase were monitored by comparing their optical emission intensities at a wavelength of 257 nm with those of SO2 at approximately 320 nm. The optimization of the HAR profiles of the CHM can be controlled by sidewall sulfurization of the CHM to obtain desirable profile shapes for the HAR features.

DOI： 10.1016/j.apsusc.2023.158876

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CiNii Research

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Environmental Technology and Innovation  

Organic fertilizers are useful in hydroponic agriculture to bring about a sustainable society with minimal pollution. Irradiation of L-tryptophan (L-Trp) solutions with electrically neutral atomic oxygen produces immediate bactericidal activity. After oxygen radical irradiation of an L-Trp-containing Escherichia coli suspension at pH 6.3 for 5 min, a colony-forming unit assay showed a 6-log reduction in the number of surviving E. coli. Kynurenine and N’-formylkynurenine were identified as irradiation products in the solution using liquid chromatography–mass spectroscopy and nuclear magnetic resonance spectroscopy. Tryptophan radicals (Trp•) are precursors of kynurenine and N’-formylkynurenine and are detected using spin-trap electron spin resonance. The bactericidal effect is mediated by central carbon metabolism via enzyme deactivation in E. coli. Enzymatic deactivation via the oxygen radical irradiation of a solution containing the amino acid L-Trp eventually resulted in bacterial death.

DOI： 10.1016/j.eti.2023.103496

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CiNii Research

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Radiation Physics and Chemistry  

Radicals produced in alanine by irradiation of 2–7 keV X-rays were investigated by ESR applications; i.e., CW-ESR, pulse-ESR and ESR imaging. The relative radical yield decreased with the decreasing photon energy and the increasing dose. The 2D imaging showed that the radical concentration at the surface was extremely low even though the absorption of X-rays exponentially decreased with the penetration depth. The depth of the radical concentration peak was almost the same as the penetration depth for the X-ray irradiation with an energy lower than 5-keV. The product formed by radical recombination was observed by an LC/MS (liquid chromatograph-mass spectrum) analysis. For the soft X-ray irradiation, many radicals will be lost by the efficient radical-radical recombination due to the higher density of the radicals, similar to the high-LET irradiation by heavy ions. The spin-spin relaxation rate (1/T2), which correlates with the radical concentration, increased by the decreasing photon energy. The values of 1/T2 for the soft X-rays were compatible to that for the heavy ions with the high-LET. Based on these observations, it is concluded that the effects of irradiation by soft X-rays are similar to high-LET irradiation.

DOI： 10.1016/j.radphyschem.2023.111304

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CiNii Research

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Plasma Medicine  

Recent research into plasma-activated solutions has unveiled their considerable potential across a range of applications, including cancer treatment, industrial processes, and environmental management. This review summarizes key findings from recent studies on the effects of plasma-activated solutions, focusing on their ability to induce cell death in glioblastoma cells, enhance ethanol production in yeast, and convert organic compounds into environmentally friendly substances. The review highlights the mechanisms by which plasma-activated solutions exert their effects, such as oxidative stress induction and cellular metabolic alterations. Addition-ally, it discusses the implications of these findings for overcoming challenges in cancer therapy, improving agricultural practices, and developing novel environmental technologies. The ongoing advancements in plasma technology offer promising avenues for future research and applications, underscoring its transformative potential in both scientific and practical domains.

DOI： 10.1615/PlasmaMed.v14.i1.50

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：IFMBE Proceedings  

Low-temperature plasma (LTP) is a promising tool that can assist in cancer treatment. Plasma-treated liquids have shown a selective cytotoxic effect on cancer cells attributed to reactive species formed in discharge, but this mechanism is not completely understood. In this study, the chemical compounds formed by plasma irradiation of Ringer’s lactate solutions and their effects on non-tumorigenic breast epithelial cells (MCF-10A) and breast cancer cells (MCF-7) were investigated. Among these compounds, glyceric acid increased the cell viability by more than two-fold compared to the control samples for MCF-10A and MCF-7 cells, whereas the tricarballylic acid had a pronounced cytotoxic effect on the cells when incubated with solutions of 0.6 mM to 50 mM concentrations. A good selectivity in killing the cancer cells was observed when the chemical compounds identified in plasma-treated liquids (such as ethyl acetate, glyceric acid, and tricarballylic acid) were used in a mixture solution of a certain concentration. The results show that the LTP-generated chemical compounds have both, stimulatory and inhibitory effects on cell viability, and the best selectivity is achieved only when these compounds are combined in a certain amount and have a synergistic effect, completely killing only the cancer cells.

DOI： 10.1007/978-3-031-62523-7_17

Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Applied Surface Science  

In semiconductor device fabrication, the feature profiles of a high-aspect-ratio (HAR) Si trench is needed to be controlled considering aspect-ratio-dependent etching (ARDE). This is achieved by a cyclic process in which Ar plasma is sustained while C4F8 and SF6 are alternately injected and a short-period supply of a substrate bias is provided. Presently, the transient behaviors of gaseous and surface reactions are dynamically revealed by measuring the plasma parameters using a surface wave probe and optical emission spectroscopy. When the etched surface is fluorinated during the cycle, an ARDE-free Si-trench feature profile can be fabricated by controlling the bias-supply timing.

DOI： 10.1016/j.apsusc.2023.157981

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Applied Physics Letters  

The surface conductivity influences the etched pattern profiles in the plasma process. In the dielectric film etching, it is vital to reduce the charging build-up, which bends the trajectory of incoming ions for highly anisotropic etching. A significant increase in surface electric conductivity of SiO2 films was observed when exposed to down-flow plasmas containing hydrogen fluoride (HF) at cryogenic temperature (−60 °C). This phenomenon can be attributed to two factors: (i) the absorption of HF and/or its compounds and (ii) the presence of H2O, which is likely originating from the etching by-product of SiO2 and/or within the reactor. Comparing the surface electric resistance of the samples treated with HF plasmas to that of CF4/H2 and C4F8/H2 plasmas, we found that HF plasma treatment enables to be approximately three and six orders of magnitude lower. By using in situ x-ray photoemission spectroscopy, it was revealed that the presence of HF and/or its compounds and H2O were absorbed on the sample surface at −60 °C. These results strongly suggest that the cryogenic plasma etching with HF-contained gases can be used to alleviate the charge build-up issues.

DOI： 10.1063/5.0173553

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CiNii Research

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Japanese Journal of Applied Physics  

Metal-organic CVD (MOCVD) is a well-established means of epitaxial growth of III-nitrides in terms of production. To overcome the drawbacks of MOCVD, we have developed a radical-enhanced MOVCVD (REMOCVD) technique which is promising to grow group-III nitride materials at lower temperatures without ammonia gas. The gas phase behavior of trimethyl gallium (TMG) and triethyl gallium (TEG) in the chamber is studied with optical emission spectroscopy (OES) and quadrupole mass spectroscopy. From OES results, it is found that the parasitic reactions due to activated Ga and CN could be avoided by introducing hydrogen as a source gas together with nitrogen gas. The TEG is completely decomposed in REMOCVD at 550 °C which is a much lower temperature compared to TMG in a hydrogen atmosphere. Also, it is found that due to the low decomposition temperature of TEG, TEG contaminated the gas line which needs to be cleaned often.

DOI： 10.35848/1347-4065/acfd34

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CiNii Research

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Plasma Processes and Polymers  

In-liquid plasma (ILP) process has been an attractive route for nanomaterial synthesis due to its high-yield production in low-temperature atmospheric pressure conditions. In comparison with conventional ILP synthesis that produces free-standing nanomaterials, this work brings a new perspective on the application of the ILP process through carbon formation directly on ethanol-immersed two-dimensional (foil) and three-dimensional (3D) (foam) metal substrates. Three types of carbon, including graphene, graphitic carbon, and amorphous carbon, were simultaneously produced during plasma discharge. Graphitic and amorphous carbon formed radially and coexisted on the metal substrate surface, while free-standing graphene was produced in ethanol. A conformal coating was achieved on the exterior surface of the 3D-networked substrate. The proposed mechanism for carbon formation on metal substrates is presented here.

DOI： 10.1002/ppap.202300036

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CiNii Research

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Japanese Society for Thermal Medicine  

<p>Low temperature plasma (LTP) has been proposed as a novel therapeutic method for its anti-cancer potential. However, its biological effects in combination with other physical modalities remain to be elusive. Therefore, this study was aimed to determine the effects of low temperature helium plasma (He-LTP) in combination with mild hyperthermia (HT, 42℃ for 20 min). Human lymphoma U937 cells were exposed to HT, immediately after He-LTP treatment. He-LTP in combination with HT showed enhanced cell death, which was accompanied by increased intracellular reactive oxygen species (ROS) production. These findings suggest that He-LTP can enhance the apoptotic effects of mild HT due to the increased in intracellular ROS generation as He-LTP has been known to caused marked induction of ROS in the aqueous medium. These findings would be helpful when establishing a therapeutic strategy for LTP in combination with mild HT. Here, the biological effects of LTP, and the combination with hyperthermia and LTP or LTP -activated solutions for cancer therapy have been summarized in this review.</p>

DOI： 10.3191/thermalmed.39.21

CiNii Research

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Japanese Journal of Applied Physics  

The characteristics of a gas-temperature-controllable atmospheric-pressure helium plasma jet and the development of an experimental system for cell viability assays of yeasts (fission yeast Schizosaccharomyces pombe and budding yeast Saccharomyces cerevisiae) are reported. The physicochemical properties of the plasma plume, which can maintain the temperature of the irradiated object at a temperature suitable for yeast, were not significantly different from those of a typical helium plasma jet. Furthermore, good reproducibility of cell viability was observed when gas temperature, gas flow rate, applied high voltage, and irradiation distance remained fixed, and only irradiation time was used as a parameter. This experimental system allows us to carry out various experiments, such as the search for plasma-resistant mutants that will contribute to the identification of genes involved in resistance to direct plasma irradiation.

DOI： 10.35848/1347-4065/acd4ca

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Plasma Processes and Polymers  

Lactate is used in the food and pharmaceutical industries and is a crucial intermediate for synthesis. Plasma-activated lactate (PAL) in Ringer's solution was recently shown to have effective antitumor action. Small molecule aldehydes, ketones, and organic acids were produced from lactate during plasma exposure, and five-membered conjugated lactone isomers of furanone (C5H6O2) were detected formed by interactions of lactate or its fragments with •OH, organic radicals, and H2O2. 2,3-Dimethyl-tartaric acid may be the effective component in PAL for the selective killing of cancer but not normal cells and possible pathways for its synthesis are provided. Aqueous reaction mechanisms are explained, including dehydration, esterification, hydrolysis, and dimerization. This study will help develop novel cancer therapies and further plasma organic chemistry.

DOI： 10.1002/ppap.202200193

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：ACS Measurement Science Au  

Considering the challenges in isolating circulating tumor cells (CTCs) pertaining to cellular stress and purity, we report the application of a blood microfiltration device as an optimal approach for noninvasive liquid biopsy to target CTCs. We experimentally analyzed the filtration behavior of the microfilter using pressure sensing to separate tumor cells from leukocytes in whole blood. This approach achieved an average recovery of >96% of the spiked tumor cells and depletion of >99% of total leukocytes. Furthermore, we carried out genomic profiling of the CTCs using the blood microfiltration device. The method was also applied in a clinical setting; DNA amplification was performed using a small number of microfiltered CTCs and epidermal growth factor receptor mutations were successfully detected to characterize the efficacy of molecularly targeted drugs against lung cancer. Overall, the proposed method can provide a tool for evaluating efficient filtration pressure to concentrate CTCs from whole blood.

DOI： 10.1021/acsmeasuresciau.2c00057

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PubMed

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Vacuum  

The effects of substrate temperature (Ts) on the etch rate (ER) of the PECVD-prepared SiN, SiO2 and amorphous carbon (a-C) films, and their selectivity were investigated with a CF4/H2 plasma. The ERs for the SiN at all Ts were higher than that for the SiO2 films. As Ts was decreased from 50 to −20 °C, the ER for the SiN decreased. Contrarily, the ER of the SiO2 films increased. The etching selectivity of SiN over SiO2 reached to near unity when the Ts was −20 °C. At the same time, the ER of for the a-C films was found to be around 0.1 nm/s and irrespective of Ts. The fluorocarbon (FC) thickness was greater for the SiO2 films than that of the SiN. The lower ER for the SiO2 was therefore attributed to the thicker FC layer and resultant etching mechanism. As the Ts was decreased, the FC thickness on the SiO2 films decreased, which led to the ER decrease. The decrease of ER for the SiN etching at the low temperature was likely due to the higher stability of the surface N–H modification layer, compared with that processed at 20 °C, which was confirmed by the in situ FTIR.

DOI： 10.1016/j.vacuum.2023.111863

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CiNii Research

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Scientific Reports  

Various liquid biopsy methods have been developed for the non-invasive and early detection of diseases. In particular, the detection of circulating tumor cells (CTCs) and cancer-associated fibroblasts (CAFs) in blood has been receiving a great deal of attention. We have been developing systems and materials to facilitate such liquid biopsies. In this study, we further developed glass filters (with various patterns of holes, pitches, and non-adhesive coating) that can capture CTCs, but not white blood cells. We optimized the glass filters to capture CTCs, and demonstrated that they could be used to detect CTCs from lung cancer patients. We also used the optimized glass filters for detecting CAFs. Additionally, we further developed a system for visualizing the captured cells on the glass filters. Finally, we demonstrated that we could directly culture the captured cells on the glass filters. Based on these results, our high-performance glass filters appear to be useful for capturing and culturing CTCs and CAFs for further examinations.

DOI： 10.1038/s41598-023-31265-9

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Free Radical Research  

This review provides a description of the historical background of the development of biological applications of low-temperature plasmas. The generation of plasma, methods and devices, plasma sources, and measurements of plasma properties, such as electron dynamics and chemical species generation in both gaseous and aqueous phases, were assessed. Currently, direct irradiation methods for plasma discharges contacting biological surfaces, such as the skin and teeth, are related to plasma biological interactions. Indirect methods using plasma-treated liquids are based on plasma–liquid interactions. The use of these two methods is rapidly increasing in preclinical studies and cancer therapy. The authors address the prospects for further developments in cancer therapeutic applications by understanding the interactions between the plasma and living organisms.

DOI： 10.1080/10715762.2023.2230351

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Free Radical Research  

We investigated the effect of cold plasma application on the yield and grain quality of rice (Oryza sativa L.), focusing on the brewer’s rice cultivar, Yamadanishiki. Two treatment methods were examined in a paddy; direct plasma irradiation of seedlings and indirect treatment with plasma-activated Ringer’s lactate solution (PAL) during the vegetative growth phase. Periodic direct irradiation for 30 s increased whole plant weight and grain yield. Treatment with PAL promoted some growth of panicles relatively and partially suppressed the growth of culms and leaves. Both treatments affected the grain quality; an increase of the ratio of white-core grains to total number of grains, which is suited for producing Japanese sake rice, as well as a decrease of the ratio of immature grains. The results showed that the effective production of rice grains for sake production can be improved by the application of cold plasma treatment of rice seedlings in a paddy.Highlight Rice plants of brewer’s rice cultivar in a paddy were treated with cold plasma, by the direct irradiation of plants and the immersed of plants in plasma-activated Ringer’s lactate (PAL). Direct plasma irradiation promoted plant weight, grain ripening, and increased yield. PAL treatment affected the growth of main stem and promoted the growth of panicles relatively. Both treatments improved the producing white-core grains, in addition to promotion of grain ripening. Cold plasma treatment can be applied to produce stable and high-quality food in various agriculture and food industries, which can achieve the sustainable developmental goals (SDGs).

DOI： 10.1080/10715762.2023.2215914

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Free Radical Research  

Cold atmospheric pressure plasmas are promising medical tools that can assist in cancer treatment. While the medical pathology mechanism is substantially understood, knowledge of the contribution of reactive species formed in plasma and the mode of activation of biochemical pathways is insufficient. Herein, we present a concept involving antitumoral plasma-activated organics, which is envisaged to increase cytotoxicity levels against cancer cells. Ringer′s acetate solution was irradiated by low-temperature plasma at atmospheric pressure and possible reaction pathways of the compound generation are presented. The chemical compounds formed by plasma treatment and their effects on non-tumorigenic breast epithelial cells (MCF-10A) and breast cancer cells (MCF-7) were investigated. The cell viability results have shown that plasma-derived compounds have both, stimulatory and inhibitory effects on cell viability, depending on the concentration of the generated compounds in the irradiated liquids. Previous studies have shown that oxidative stresses involving reactive oxygen and nitrogen species (RONS) can be used to kill cancer cells. Hence, while RONS offers promising first-step killing effects, cell viability results have shown that plasma-derived compounds, such as acetic anhydride and ethyl acetate, have the potential to play important roles in plasma-based cancer therapy.

DOI： 10.1080/10715762.2023.2201390

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PubMed

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Sains Malaysiana  

Papaya is a one of the important tropical fruit crops with a global export of 353 ktonnne reported in 2020. The germination of papaya seed is erratic and often non-uniform. Plasma assisted priming of seed was performed at atmospheric pressure in a parallel plate dielectric barrier discharge system. The germination rate of papaya seeds and the growth performance of the seedling were monitored for several treatment plans combining the atmospheric pressure plasma treatment with soaking of seed in deionized water. An enhanced germination rate of 92% was obtained by the plasma assisted priming, compared to the untreated of 60%. The plasma assisted priming performed by plasma treatment and soaking in an opposite sequence showed different requirement and possibly involved different mechanisms. The treatment time was reduced to only 4 minutes for pre-soaked seeds, otherwise the germination rate increased with the plasma treatment time from 3 to 30 min treatment. The plasma assisted priming approaches were also found enhancing seedling growth performance. The treated seedling grows about two times bigger and the dried mass measured after 30 days was more than 100% compared to that of the untreated and hot water treated seeds.

DOI： 10.17576/jsm-2023-5202-21

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Language：English   Publishing type：Research paper (scientific journal)  

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Language：English   Publishing type：Research paper (scientific journal)  

Web of Science

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Journal of Applied Physics  

Damage-free atomic layer etching (ALE) of GaN was demonstrated using a cyclic process in which the chlorinated layer formed by Cl2 plasma exposure was removed by exposure to Ar plasma with energy-controlled ions when the substrate temperature was maintained at 400 °C. The layer chlorinated at 400 °C by Cl2 plasma exposure was found to be thinner than that chlorinated at 25 °C. Therefore, in the case of an Ar+-ion energy of 70 eV, the "ALE synergy"parameter, which quantifies the degree to which a process approaches the ideal ALE regime, decreased from 86% at a substrate temperature of 25 °C to 24% at a substrate temperature of 400 °C. A substrate temperature of 400 °C promoted etching even at the lower ion energy of 40 eV, thereby resulting in a higher ALE synergy of 62%. The vertical etching profile with no degradation of photoluminescence near the band edge on the etched surface was then observed. The proposed high-temperature ALE method is promising for realizing a vertical pattern profile via damage-free etching of GaN.

DOI： 10.1063/5.0131685

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Materials Science and Engineering: A  

The unique structural properties of vertically aligned graphene sheets or Carbon Nanowalls (CNWs) have attracted great interests for their potential for various applications in microelectronic devices, energy storage, and catalyst support materials. During the handling or operation of the devices, tension and/or pressure are often needed. Under such conditions, CNWs must undergo compression and stress. Therefore, the deformation mechanism and evolution behavior of the CNW structures under load play a critical role in the performance and reliability of the devices. In this study, the mechanical properties of a typical maze-like CNW structure synthesized by a Radial Injection Plasma Enhanced Chemical Vapor Deposition (RI-PECVD) technique were analyzed by employing the nanoindentation method. The measured compressive strength of the CNW structure was 50 MPa with an average modulus E value of ∼28 GPa, which is significantly higher than that of pyrolytic graphite and other graphene-based materials such as 3D graphene-derived carbon, commercial graphene, and reduced graphene oxide films. An elastoplastic behavior of a soft material was observed in high-resolution microscopy and a mechanism of deformation for CNWs is elucidated.

DOI： 10.1016/j.msea.2022.144428

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Genes and Environment  

Background: Non-thermal atmospheric pressure plasma technologies form the core of many scientific advances, including in the electronic, industrial, and biotechnological fields. The use of plasma as a cancer therapy has recently attracted significant attention due to its cancer cell killing activity. Plasma-activated Ringer’s lactate solution (PAL) exhibits such activity. In addition to ROS, PAL contains active compounds or species that cause cancer cell death, but the potential mutagenic risks of PAL have not been studied. Results: PAL has a low pH value and a high concentration of H2O2. H2O2 was removed from PAL using catalase and catalase-treated PAL with a pH of 5.9 retained a killing effect on HeLa cells whereas this effect was not observed if the PAL was adjusted to pH 7.2. Catalase-treated PAL at pH 5.9 had no significant effect on mutation frequency, the expression of γH2AX, or G2 arrest in HeLa cells. Conclusion: PAL contains one or more active compounds or species in addition to H2O2 that have a killing effect on HeLa cells. The compound(s) is active at lower pH conditions and apparently exhibits no genotoxicity. This study suggested that identification of the active compound(s) in PAL could lead to the development of novel anticancer drugs for future cancer therapy.

DOI： 10.1186/s41021-023-00260-x

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Frontiers in Physics  

DOI： 10.3389/fphy.2022.1118018

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Free Radical Research  

Low-temperature plasma (LTP) has been widely used in life science. Plasma-activated solutions were defined as solutions irradiated with LTP, and water, medium, and Ringer’s solutions have been irradiated with LTP to produce plasma-activated solutions. They contain chemical compounds produced by reactions among LTP, air, and solutions. Reactive oxygen and nitrogen species (RONS) are major components in plasma-activated solutions and recent studies revealed that plasma-activated organic compounds are produced in plasma-activated Ringer’s lactate solution (PAL). Many in vitro and in vivo studies demonstrated that PAL exhibits anti-tumor effects on cancers, and biochemical analyses revealed intracellular molecular mechanisms of cancer cell death by PAL.

DOI： 10.1080/10715762.2023.2182663

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Japanese Journal of Applied Physics  

Silicon carbide (SiC) was coated onto carbon nanowall (CNW) scaffolds using chemical vapor deposition with a vinylsilane precursor at 700 °C to investigate the influence of the wall edge width, wall-to-wall distance, and surface morphology. The wall edge width ranged from 10 nm to those filling the wall-to-wall space without disrupting the CNW morphology. When SiC-coated CNWs (SiC/CNWs) were used as scaffolds for cell culture, cell viability increased until the edge area ratio reached 40%. In over 40% of edge area ratio, cell viability was saturate and comparable to flat surfaces such as SiC films on the Si substrate (SiC/Si) and control samples prepared using polystyrene. Calcification was suppressed in the CNWs, SiC/CNWs, and SiC/Si scaffolds compared to polystyrene. Our results suggest that SiC-coated CNW scaffolds could suppress calcification and promote cell proliferation.

DOI： 10.35848/1347-4065/ac9319

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Japanese Journal of Applied Physics  

Low-temperature plasma-processing technologies are essential for material synthesis and device fabrication. Not only the utilization but also the development of plasma-related products and services requires an understanding of the multiscale hierarchies of complex behaviors of plasma-related phenomena, including plasma generation in physics and chemistry, transport of energy and mass through the sheath region, and morphology- and geometry-dependent surface reactions. Low-temperature plasma science and technology play a pivotal role in the exploration of new applications and in the development and control of plasma-processing methods. Presently, science-based and data-driven approaches to control systems are progressing with the state-of-the-art deep learning, machine learning, and artificial intelligence. In this review, researchers in material science and plasma processing, review and discuss the requirements and challenges of research and development in these fields. In particular, the prediction of plasma parameters and the discovery of processing recipes are asserted by outlining the emerging science-based, data-driven approaches, which are called plasma informatics.

DOI： 10.35848/1347-4065/ac9189

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Nanomaterials  

Surface-assisted laser desorption/ionization mass spectrometry (SALDI-MS) is performed using carbon nanowalls (CNWs) for ionization-assisting substrates. The CNWs (referred to as high-quality CNWs) in the present study were grown using a radical-injection plasma-enhanced chemical vapor deposition (RI-PECVD) system with the addition of oxygen in a mixture of CH4 and H2 gases. High-quality CNWs were different with respect to crystallinity and C–OH groups, while showing similar wall-to-wall distances and a wettability comparable to CNWs (referred to as normal CNWs) grown without O2. The efficiency of SALDI was tested with both parameters of ion intensity and fragmental efficiency (survival yield (SY)) using N-benzylpyridinuim chloride (N-BP-CI). At a laser fluence of 4 mJ/cm2, normal CNWs had an SY of 0.97 and an ion intensity of 0.13, while 5-sccm-O2– high-quality CNWs had an SY of 0.89 and an ion intensity of 2.55. As a result, the sensitivity for the detection of low-molecular-weight analytes was improved with the high-quality CNWs compared to the normal CNWs, while an SY of 0.89 was maintained at a low laser fluence of 4 mJ/cm2. SALDI-MS measurements available with the high-quality CNWs ionization-assisting substrate provided high ionization and SY values.

DOI： 10.3390/nano13010063

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Proceedings of SPIE - The International Society for Optical Engineering  

There has been considerable interest in the development of isotropic atomic layer etching (ALE) for the conformal removal of thin films. Material selectivity is crucial for the development of isotropic ALE because the next generation of semiconductor devices will be constructed with miniaturized 3D structures using a variety of very thin films. We developed plasma-assisted thermal-cyclic ALE, which is a repetition of surface modification by plasma exposure and removal of the modified surface by infrared heating. We developed a 300-mm tool, namely, dry chemical removal (DCR), which is equipped with an inductively coupled plasma (ICP) source and infrared lamps, to facilitate rapid thermal desorption of the modified surface. An important feature of the plasma-assisted thermal-cyclic ALE is that it has more tuning knobs than that of conventional ALE because it uses two temperatures: a low temperature for surface modification and an elevated temperature for the removal of the modified surface. This paper presents the selective ALE of various materials, i.e., Si3N4, TiN, W, and SiGe using the developed tool. The mechanisms of the selectivity are divided into two categories: formation of an ammonium salt-based modified layer and selectivity control by adjusting the infrared heating time. This paper reviews the selective ALE mechanisms, focusing on the results of in situ analysis of surface reactions, and presents some of the latest findings.

DOI： 10.1117/12.2664547

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Language：English   Publishing type：Research paper (scientific journal)  

CiNii Research

Language：English   Publishing type：Research paper (scientific journal)  

CiNii Research

Language：English   Publishing type：Research paper (scientific journal)  

CiNii Research

Language：English   Publishing type：Research paper (scientific journal)  

CiNii Research

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Chinese Physics B  

The seed of Carica papaya consists of a hard shell-like testa with inhibitors in vivo causing slow, erratic and asynchronous germination. In this work, plasma-activated water prepared by microsecond-pulsed plasma jets (μPAW) was applied to treat papaya seeds. The μPAW after plasma activation of 30 min was about 40 °C. The reactive species such as NO2, NO3, and H2O2 in the μPAW activated from deionized water were measured and correlated to the seed germination rate and the seedling growth performance. The μPAW-treated papaya seed achieved a higher germination rate of 90%, which is 26% higher than the control group using deionized water. Comparing the results with a hot water (40 °C) reference group showed that the reactive species in μPAW played primary roles in germination improvement, with little effect caused by the heat shock. The μPAW also sterilized the treated seeds, reducing the germination stress. The morphological change in the seeds was observed by SEM, showing an effect of physical etching after treatment promoting seed imbibition. The biochemical mechanism of the seed germination was deduced with reference to the evolution of surface chemistry, functional groups, and ABA content. The accelerated seed metabolism observed was corresponded to the chemical modification pathway. Besides, early seedlings developed from treated seeds were observed to be healthy, grow more leaves, and have better root structures. The content of MDA in the treated papaya seedlings decreased along with increased SOD and higher ion concentration. The μPAW that can be prepared at atmospheric pressure for bulk production offers a low-risk and cost-effective seed priming technology that may significantly increase the production of agricultural crops.

DOI： 10.1088/1674-1056/ac904e

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Coatings  

Heel marks (HMs), which are the black stains made by shoe soles on indoor floors, can be difficult to remove. However, this study shows how spark discharges combined with pressurized airflow in 60 s discharge treatments can remove such HMs. We further show that maximizing the HM removal rates depended on the electrode gap distance because of changes in the spark discharge parameters. In our experiments, the electrical voltage waveforms are shown with voltage spikes, called spark discharges, and the spike numbers were counted in 0.6-ms time units. It was found that the number of spark discharges increases when the electrode gap distance was widened from 5 mm to 10 mm and the pressurized airflow was added, and the HM removal rates increased 11.5%, the HM removal rates could be maximized. Taken together, the results show that spark discharges combined with pressurized air can remove HMs from indoor floors without no visual damage. This paper is a preliminary report showing that HMs can be removed by plasma.

DOI： 10.3390/coatings12121938

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Scientific Reports  

Dry etching of ternary metal carbides TiAlC has been first developed by transferring from wet etching to dry etching using a floating wire (FW)-assisted Ar/ammonium hydroxide vapor plasma. FW-assisted non-halogen vapor plasma generated at medium pressure can produce high-density reactive radicals (NH, H, and OH) for TiAlC surface modifications such as hydrogenation and methylamination. A proposed mechanism for dry etching of TiAlC is considered with the formation of the volatile products from the modified layer.

DOI： 10.1038/s41598-022-24949-1

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：ACS Applied Materials and Interfaces  

Although hexagonal boron nitride (hBN) is a thermally conductive and electrically insulating filler in composite materials, surface modification remains difficult, which limits its dispersibility and functionalization. In this study, carbon layer formation on hBN particles by plasma processing in hydroquinone aqueous solution was investigated as a surface modification technique. Carbon components with features of polymeric hydrogenated amorphous carbon were found to be uniformly distributed on the hydroquinone-aided plasma-modified hBN (HQpBN) particles. Electron spin resonance measurements revealed abundant unpaired electrons in HQpBN, indicating that defects were formed on hBN by plasma processing and that the carbon layer contained dangling bonds. The defects on hBN could help in the attachment of the carbon layer, whereas the dangling bonds could act as reactive sites for further functionalization. The carbon layer on HQpBN was successfully functionalized with isocyanate groups, thus confirming the ability of this carbon layer to facilitate surface modification. These results demonstrate that the carbon layer formed on hBN can provide a designable interface in organic/inorganic composite materials.

DOI： 10.1021/acsami.2c15951

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Vacuum  

In the growth of hydrogenated amorphous carbon (a-C:H) films by plasma enhanced chemical vapor deposition (PECVD) with H2, CH4 and C3H6 plasma, the gas phase reaction of active species and their contribution to properties of deposited a-C:H film were quantitatively investigated using appearance quadrupole mass spectrometry (QMS) and machine learning. The QMS measurement indicated that two-types of neutral radicals were generated by the dissociation and polymerization of the raw material gasses. A random forest regression model was employed as a prediction model to analyze the correlation between the neutral species and etching rates by molecular oxygen (O2) plasma without any stage bias, which were measured by in-situ ellipsometry. The coefficient of determination (R2), an indicator of the degree of prediction accuracy, was 0.906 and 0.584 for the training and test data, respectively. SHapley Additive exPlanations (SHAP), interpreting the random forest model, were used to quantitatively indicate the contribution of radicals to the etching rate, including their synergistic and secondary effects. They indicated that carbon-rich radicals, such as C3H3 and C5H5, contributed to a decrease in the etching rate, whereas hydrogen-rich radicals, such as CHx (x=1,2,3,4), C2H5, C4H9, and C5H9,11 induced an increase in the etching rate by the O2 plasma. (200 words)

DOI： 10.1016/j.vacuum.2022.111351

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Japanese Journal of Applied Physics  

Progress in computational methods and personal computing has made possible more accurate estimations for primary dissociation channels and energies. The main dissociation route is revealed to be via the 7E excited state with an energy of 12.23 eV, which is composed of transitions from the highest occupied molecular orbital with b1 symmetry to some degenerate unoccupied e molecular orbitals. The main contributing e orbitals consisted of antibonding combination of C2F4 π-bonding orbitals. This degenerate 7E state is lowered by non-adiabatic transitions through the conical interactions on the dissociating route to 2C2F4, so the energy is finally relaxed at the dissociative second lowest 1E excited state leading to 2C2F4 production. In the electron attachment process, the calculated results show that the F- ion is produced from the excited states of the D4h c-C4F8- ion through conical interactions at the energies of 4.3 eV, 5.6 eV, and 5.0 eV, along the C-F dissociation route.

DOI： 10.35848/1347-4065/ac895e

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Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Plasma Processes and Polymers  

Flake-shaped carbon nanomaterials with nitrogen (N) and iron (Fe) addition, so-called carbon nanoflakes (CNFLs), were synthesized by the in-liquid plasma using two different kinds of additive agents, such as hemin and iron (II) phthalocyanine (FePc). According to scanning electron microscopy images and Raman spectra, CNFLs with a size of at least 100 nm order were formed regardless of types of additive agents, and crystallinity of six-membered ring structures was improved as additive agents increased. Photoelectron spectra showed that pyridinic N contents increased from 1.05% to 2.02% with increasing FePc, while those decreased from 0.34% to 0.14% with hemin. In the oxygen reduction reaction, onset potential values also increased from 0.71 to 0.79 eV with increasing FePc, while those decreased from 0.60 to 0.47 eV with hemin. These results suggested that the catalytic activity of CNFLs was effectively improved by the increase of pyridinic N by the in-liquid plasma synthesis with FePc. In contrast, the electron transfer numbers reached 3.81 when hemin increased, although those were less than 2.88 in the cases using FePc. These results mean that the in-liquid plasma synthesis method of CNFLs using FePc has the potential to further improve its catalytic activity.

DOI： 10.1002/ppap.202100203

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Japanese Journal of Applied Physics  

DOI： 10.35848/1347-4065/ac6726

Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Physical Chemistry Chemical Physics  

We consider the corona model and local thermal equilibrium approximations of a real plasma to measure the electron temperature (Te) and density (ne), respectively, using the optical emission spectroscopy (OES) method in dual-frequency pulsed capacitively coupled plasmas (CCPs) in a reactive mixture of Ar/O2/C4F8 at a low operating pressure. The operation conditions such as DC continuous and synchronized were used for the study and plasma characterization for the intended plasma application such as high aspect ratio etching (HARE). We show that the present plasma conditions are dominated by a corona balance rather than the supremacy of multi-step excitation. This fact has enabled us to utilize the modified Boltzmann plot technique to evaluate the Te values. In the second method, we simultaneously used the Boltzmann and Saha equations to determine the ne value using the line intensity ratio and the value of Te. Time-resolved measurements of Te and ne were performed for completeness, and the insight of the pulsed discharge was investigated. Time evolution of ne and Te using the OES method revealed a similar trend in the change of plasma parameters, indicating electron impact ionization during the pulse on phase. It was seen that ne in the afterglow speedily decreased within a short time of ∼5 μs. Analysis suggests the formation of afterglow plasmas, which are composed of positive and negative ions with very low electron density. The results revealed that the DC-synchronized operation could be useful for plasma application such as HARE due to different plasma characteristics. It also suggests the production of ion-ion plasmas by the effective utilization of negative ions in the afterglow phase. The corona balance condition was validated in our experiments, and the results were compared with the existing literature.

DOI： 10.1039/d2cp00289b

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PubMed

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Plasma Processes and Polymers  

Reduction of SnO2 to form spherical Sn particles and Sn etching are obtained by floating wire (FW)-assisted medium-pressure H2/Ar plasma. High-density H2/Ar plasma (1014 cm−3) with a larger treatment area at medium pressure (10 kPa) produces a two-times higher removal rate of SnO2 (0.111 mg/min) than that at atmospheric pressure with the same treatment area of 300 mm2. SnO2 film is removed from the glass surface by a two-step process involving (1) reduction of SnO2 by FW-H2/Ar plasma to form spherical Sn particles and (2) removal of low-contact Sn particles by water-based cleaning. High surface smoothness (roughness of 0.488 nm) and high optical transmittance (>92%) of treated samples indicate no damage compared to that of pristine quartz glass.

DOI： 10.1002/ppap.202100209

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Applied Physics Express  

Ringer's lactate solution was irradiated with non-equilibrium plasma under airtight conditions. The plasma-activated lactate (PAL) was produced with argon, oxygen, and nitrogen gases following purging of Ar. Cytotoxicity could be controlled by diluting PAL, and a killing effect was selectively obtained on cancer cells compared to normal cells for Ar+O2+N2 PALs. Nonetheless, cytotoxicity was partly reproduced by similar concentrations of H2O2 and NO2- in the PALs. The organics produced by plasma irradiation to lactate were investigated using nuclear magnetic resonance, and the generation of methyl amino species was confirmed.

DOI： 10.35848/1882-0786/ac6360

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Journal of Vacuum Science and Technology B  

Plasma-assisted thermal-cyclic atomic-layer etching (ALE) of tungsten (W), the selectivity of which with respect to TiN can be tuned between highly selective and nonselective by changing infrared-heating time, has been demonstrated. It is a two-step process consisting of exposure to radicals generated in a CHF3/O2 or CH2F2/O2/Ar plasma followed by infrared heating. Analysis by in situ x-ray photoelectron spectroscopy confirmed that a WFx-based modified surface formed on the surface of a W film exposed to radicals at -22 °C. The modified surface on the W film is volatile at a heating temperature lower than that required for removing the modified surface on the TiN film. Cyclic etching of both W and TiN was performed by using the CH2F2/O2/Ar plasma and infrared heating in a 300-mm ALE apparatus. When the infrared-heating time was not long enough to remove the modified surface on TiN, the cyclic repetition etched only the W film. On the other hand, when the infrared-heating time was long enough to remove modified surfaces on both W and TiN, the cyclic repetition etched both W and TiN films. Therefore, both highly selective and nonselective ALEs for W and TiN were obtained by choosing an optimum infrared-heating time. This shows that material selectivity in plasma-assisted thermal-cyclic ALE can be controlled by changing the infrared-heating time.

DOI： 10.1116/6.0001660

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：AIP Advances  

Carbon nanowalls (CNWs) with average wall-to-wall distances ranging from 100 to 3300 nm were synthesized using a radical injection plasma-enhanced chemical vapor deposition system. Application of a negative high voltage to the growth substrate using an inductor energy storage (IES) circuit provided CNWs with wall-to-wall distances depending on the nano-second pulse voltage of the IES circuit. Sparse isolated CNWs with average wall-to-wall distances of 700 nm were used for culturing Saos-2 cells. These cells showed better adhesion than the control after 2 days’ incubation and enhanced gene expression of the osteogenic differentiation genes Runt-related transcription factor 2 (Runx2) and osteocalcin after 10 days’ incubation. Sparse isolated CNW scaffolds hold promise for regulating the differentiation of osteoblast-like cells.

DOI： 10.1063/5.0075530

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Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Japanese Journal of Applied Physics  

Ethanol production by budding yeast was compared between direct and indirect plasma irradiation. We observed enhancement of ethanol production and cell growth not by indirect plasma irradiation but by direct plasma irradiation. Glucose consumption was increased in budding yeast by direct plasma irradiation. Extracellular flux analysis revealed that glycolytic activity in the budding yeast was elevated by direct plasma irradiation. These results suggest that direct plasma irradiation enhances ethanol production in budding yeast by elevating the glycolytic activity.

DOI： 10.35848/1347-4065/ac2037

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Japanese Journal of Applied Physics  

Inspired by the ideas of many authors, we provide insight on state-of-the-art potential technologies for the prevention and prediction of infectious diseases before they spread. This review also surveys virus sterilization with ultraviolet light and low temperature plasma technologies. Researchers in the various fields of medicine, materials, electronics, and plasma sciences have addressed increasingly challenging demands and the discussion encompasses the major challenges in societies that are faced with the threat of infectious diseases. In addition, technologies that use nanomaterials are evaluated for infection prevention and hygiene purposes. Advances in biomedical diagnostics for health care in terms of complementary metal-oxide-semiconductor transistors-based devices and telemetry for health monitoring are also reviewed.

DOI： 10.35848/1347-4065/ac1c3d

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Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Japanese Journal of Applied Physics  

Reactive nitrogen species (RNS) generated by controlled electron impacts in conjunction with the use of dinitrogen can react with oxygen and/or hydrogen to generate highly reactive compounds. The related field of functional nitrogen science provides new opportunities for nitrogen utilization based on non-equilibrium plasma processing. This revolutionary technique permits plasma-based nitrogen fixation at the locations at which materials such as dopants and fertilizers are required. This system, based on the in situ generation of RNS at the point of use, is expected to replace conventional processes involving nitrogen cycles employing ammonia and nitric acid. Optimization of this new approach will require nitrogen doping to be tuned by atomic-scale localization of nitrogen. This review discusses the applications of functional nitrogen and the processes by which functionalization in both inorganic materials and living organisms can occur when using RNS.

DOI： 10.35848/1347-4065/ac3558

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Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Japanese Journal of Applied Physics  

Nitrogen is a very common element, comprising approximately 78% of Earth's atmosphere, and is an important component of various electronic devices while also being essential for life. However, it is challenging to directly utilize dinitrogen because of the highly stable triple bond in this molecule. The present review examines the use of non-equilibrium plasmas to generate controlled electron impacts as a means of generating reactive nitrogen species (RNS) with high internal energy values and extremely short lifetimes. These species include ground state nitrogen atoms, excited nitrogen atoms, etc. RNS can subsequently react with oxygen and/or hydrogen to generate new highly reactive compounds and can also be used to control various cell functions and create new functional materials. Herein, plasma-processing methods intended to provide RNS serving as short-lived precursors for a range of applications are examined in detail.

DOI： 10.35848/1347-4065/ac25dc

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Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Reviews of Modern Plasma Physics  

Applications of plasma diagnostics using vacuum ultraviolet absorption spectroscopy (VUVAS) in our studies are summarized in this article. The plasma diagnostics with absorption spectroscopy is a powerful tool for investigating behaviors of reactive species in plasma processes, because it enables us to measure the absolute density. In our group, we have focused on the clarification of reaction mechanisms of atomic species in the plasma processes, and the behaviors of atomic species generated in various process plasmas have been investigated using the VUVAS with a plasma light source. Using the VUVAS, we can investigate not only the absolute density but also surface reactions of atomic species in the plasma processes. On the other hand, in our group, the real-time monitoring of atomic species based on VUVAS has been realized in the plasma processes, and the effects of the initial state of reactor wall surface on the behaviors of atomic species in a process plasma have been quantitatively investigated. Moreover, the VUVAS has been applied to the measurements of reactive species generated by atmospheric pressure plasmas which attracts much attention because of its applications to the bio and medical research fields. These results and experimental technique used in our studies are extremely useful for the further developments of plasma processes such as etching, deposition, surface modification, bio-medical applications and so on in the future.

DOI： 10.1007/s41614-022-00075-3

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：IEEE International Symposium on Semiconductor Manufacturing Conference Proceedings  

Plasma diagnostics including electron density, temperature, neutral atomic densities of the CH4H2 plasmas were performed in a capacitively-coupled reactor using surface-wave probe, Langmuir probe and vacuum ultraviolet absorption spectroscopy. The plasma density increased monotonically with varying H2 content from 30 to 90 %. The electron temperature first decreased with H2 up to 50 % and then increased at higher H2 concentration. The HF concentration reached a maximum value at a H2 of approximately 50 %, which is probably due to balance between H and F radicals from the plasma. Increasing the H2 content resulted in a higher H concentration and a less cross-linked structure of the amorphous hydrofluorocarbon films, analyzed by using in situ Fourier transformation infrared spectroscopy.

DOI： 10.1109/ISSM55802.2022.10027112

Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Coatings  

With the increasing interest in dry etching of silicon nitride, utilization of hydrogencontained fluorocarbon plasma has become one of the most important processes in manufacturing advanced semiconductor devices. The correlation between hydrogen-contained molecules from the plasmas and hydrogen atoms inside the SiN plays a crucial role in etching behavior. In this work, the influences of plasmas (CF4/D2 and CF4/H2 ) and substrate temperature (Ts, from −20 to 50◦ C) on etch rates (ERs) of the PECVD SiN films were investigated. The etch rate performed by CF4/D2 plasma was higher than one obtained by CF4/H2 plasma at substrate temperature of 20◦ C and higher. The optical emission spectra showed that the intensities of the fluorocarbon (FC), F, and Balmer emissions were stronger in the CF4/D2 plasma in comparison with CF4/H2 . From X-ray photoelectron spectra, a thinner FC layer with a lower F/C ratio was found in the surface of the sample etched by the CF4/H2 plasma. The plasma density, gas phase concentration and FC thickness were not responsible for the higher etch rate in the CF4/D2 plasma. The abstraction of H inside the SiN films by deuterium and, in turn, hydrogen dissociation from Si or N molecules, supported by the results of in situ monitoring of surface structure using attenuated total reflectance-Fourier transform infrared spectroscopy, resulted in the enhanced ER in the CF4/D2 plasma case. The findings imply that the hydrogen dissociation plays an important role in the etching of PECVD-prepared SiN films when the hydrogen concentration of SiN is higher. For the films etched with the CF4/H2 at −20◦ C, the increase in ER was attributed to a thinner FC layer and surface reactions. On the contrary, in the CF4/D2 case the dependence of ER on substrate temperature was the consequence of the factors which include the FC layer thickness (diffusion length) and the atomic mobility of the etchants (thermal activation reaction).

DOI： 10.3390/coatings11121535

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Scopus

Authorship：Lead author,　Corresponding author   Language：Japanese   Publishing type：Research paper (scientific journal)  

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Plasma Processes and Polymers  

The dependences of etching characteristics on substrate temperature (Ts, from –20 to 50°C) of the plasma-enhanced chemical vapor deposition (PECVD) SiN films (PE-SiN) and low-pressure chemical vapor deposition (LPCVD) SiN films (LP-SiN) with CF4/H2 plasma were investigated. The Fourier-transform infrared spectroscopy shows that both film types were N–H bond-rich films, but in different hydrogen contents (PE-SiN 22.7 at% and LP-SiN 3.8 at%) from the Rutherford backscattering spectroscopy analyses. A higher hydrogen content led to a thinner fluorocarbon thickness because of the reaction between hydrogen outflux and C and N to form an HCN byproduct. The etch rates (ER) for the PE-SiN were higher than that of the LP-SiN at all Ts, due to the different FC thickness and etching mechanisms proposed. The formation of the N−Hx layer on PE-SiN at low temperature caused the decrease in ER. For the LP-SiN, the weak dependences of Ts on surface structure and ER were observed.

DOI： 10.1002/ppap.202100078

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Plasma Processes and Polymers  

Nonequilibrium atmospheric pressure plasma has enabled a variety of new applications in medicine, agriculture, and other industries. It is particularly noteworthy that plasma itself and/or plasma-activated culture medium have been shown to preferentially kill various cancer cells. We have previously developed a plasma-activated Ringer's lactate solution (PAL) for use as a new cancer treatment. In this study, behaviors of extracellular and intracellular reactive oxygen and nitrogen species in the cellular respiratory system of PAL-treated HeLa cells were investigated using an extracellular flux analyzer and a probe to measure mitochondrial membrane potential. In PAL-treated HeLa cells, extracellular hydrogen peroxide in PAL was found to be responsible for the induction of intracellular hydrogen peroxide and apoptosis, while other components in PAL are responsible for the induction of non-H2O2 intracellular ROS and non-apoptotic cell death, which should be clarified by further experiments. We believe that these are long-lived species derived from plasma-activated lactates. Furthermore, we found that the plasma-activated lactates inhibited glycolysis and the tricarboxylic acid (TCA) cycle, but not the electron transport chain in HeLa cells. These results suggest that PAL induces multiple modes of cell death, including apoptosis through hydrogen peroxide, and non-apoptotic cell death associated with the impairment of mitochondrial functions (glycolysis and TCA cycle). These findings shed light on the novel mechanism underlying plasma-activated lactate-induced cell death.

DOI： 10.1002/ppap.202100056

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Scientific Reports  

Low-temperature plasma is being widely used in the various fields of life science, such as medicine and agriculture. Plasma-activated solutions have been proposed as potential cancer therapeutic reagents. We previously reported that plasma-activated Ringer’s lactate solution exhibited selective cancer-killing effects, and that the plasma-treated L-sodium lactate in the solution was an anti-tumor factor; however, the components that are generated through the interactions between plasma and L-sodium lactate and the components responsible for the selective killing of cancer cells remain unidentified. In this study, we quantified several major chemical products, such as pyruvate, formate, and acetate, in plasma-activated L-sodium lactate solution by nuclear magnetic resonance analysis. We further identified novel chemical products, such as glyoxylate and 2,3-dimethyltartrate, in the solution by direct infusion-electrospray ionization with tandem mass spectrometry analysis. We found that 2,3-dimethyltartrate exhibited cytotoxic effects in glioblastoma cells, but not in normal astrocytes. These findings shed light on the identities of the components that are responsible for the selective cytotoxic effect of plasma-activated solutions on cancer cells, and provide useful data for the potential development of cancer treatments using plasma-activated L-sodium lactate solution.

DOI： 10.1038/s41598-021-98020-w

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PubMed

Authorship：Lead author,　Corresponding author   Language：Japanese   Publishing type：Research paper (scientific journal)  

Authorship：Lead author,　Corresponding author   Language：Japanese   Publishing type：Research paper (scientific journal)  

Language：Japanese   Publishing type：Research paper (scientific journal)  

Authorship：Lead author,　Corresponding author   Language：Japanese   Publishing type：Research paper (scientific journal)  

Language：English   Publishing type：Research paper (scientific journal)   Publisher：IEEE Transactions on Plasma Science  

Simple low-temperature pulsed power dissociation method for high resistive liquid is proposed in this article. Active high voltage rebound tailing pulse (RTP) diodes are adopted to conventional high voltage pulse power sources. In order to explain this method, the study was performed using deionized water (DIW) (high resistive >17MΩcm) electrolysis with two immersed electrodes. The forward pulses, the full-width at half-maximum (FWHM) of 400 ns and forward voltage (7 kV) with rising-up ratio (dV/dt) of 1011 V/s, were applied to the electrodes. When a 5 kV RTP diode was simply adopted to this electrical circuit and DIW load in series, the high forward voltage pulse and continuous high reverse current were applied to this circuit. Then, H2 was generated at the anode electrode and OH radical (OH) in the water vessel. Those phenomena were apparently dependent on the anode electrode area. At the beginning of the forwarded high voltage application, the circuit behaved as capacitance load with generated ions and built up charges at the interface between DIW and the electrode. Continuous rebounded high reverse voltage and highly built-up reverse recovery charges induce avalanche breakdown of RTP diode. The rebounded electrical current was found to be collected in the circuit, accompanied by the generation of hydrogen and OH, as well as the tailing current flowing at the interface as a resistive load. In consequence, we point out that rebounded electrons injected from the surrounding water to the anode electrode interface induced the water electrolysis characteristically, according to RTP-diode inserted in the circuit.

DOI： 10.1109/TPS.2021.3102639

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Language：Japanese   Publishing type：Research paper (scientific journal)   Publisher：The Japan Society of Applied Physics  

DOI： 10.11470/jsapmeeting.2021.2.0_1677

CiNii Research

Language：Japanese   Publishing type：Research paper (scientific journal)   Publisher：The Japan Society of Applied Physics  

DOI： 10.11470/jsapmeeting.2021.2.0_1693

CiNii Research

Language：Japanese   Publishing type：Research paper (scientific journal)   Publisher：The Japan Society of Applied Physics  

DOI： 10.11470/jsapmeeting.2021.2.0_120

CiNii Research

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Redox Biology  

Non-thermal plasma (NTP), an engineered technology to generate reactive species, induces ferroptosis and/or apoptosis specifically in various-type cancer cells. NTP-activated Ringer's lactate (PAL) is another modality for cancer therapy at preclinical stage. Here we found that PAL induces selective ferroptosis of malignant mesothelioma (MM) cells, where non-targeted metabolome screening identified upregulated citrulline-nitric oxide (.NO) cycle as a PAL target .NO probe detected biphasic peaks transiently at PAL exposure with time-dependent increase, which was responsible for inducible .NO synthase (iNOS) overexpression through NF-κB activation. .NO and lipid peroxidation occupied lysosomes as a major compartment with increased TFEB expression. Not only ferrostatin-1 but inhibitors for .NO and/or iNOS could suppress this ferroptosis. PAL-induced ferroptosis accompanied autophagic process in the early phase, as demonstrated by an increase in essential amino acids, LC3B-II, p62 and LAMP1, transforming into the later phase with boosted lipid peroxidation. Therefore, .NO-mediated lysosomal impairment is central in PAL-induced ferroptosis.

DOI： 10.1016/j.redox.2021.101989

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PubMed

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Applied Physics Express  

Nonequilibrium atmospheric pressure plasma (NEAPP) has the potential for a wide range of medical applications, including wound healing, blood coagulation, and malignant cell apoptosis. However, its effect on the mammalian central nervous system remains unclear. We studied histological changes in the cerebral cortex of adult rats, following irradiation of the brain surface with NEAPP. NEAPP irradiation made three laminar tissue structures and induced high proliferation of brain-resident immature cells as well as bone marrow-derived cells. These observations indicate that NEAPP irradiation induced rearrangement of cellular and tissue organization, including cell proliferation in the central nervous system in vivo.

DOI： 10.35848/1882-0786/ac03c1

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Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Plasma Sources Science and Technology  

A mechanism of hydrogen peroxide (H2O2) generation in plasma-activated lactated Ringer's solution (PAL) has been analyzed. PAL was produced by irradiating a sodium lactate solution, a class of hydroxy acid, with non-equilibrium atmospheric pressure plasma (NEAPP). The concentration of H2O2 generation was dependent on the initial lactate concentrations, which ranged from 0-28 mM. However, the generation of H2O2 was inhibited by higher lactate concentration. The formation of H2O2 is proposed by catalyzed lactate and radicals in aqueous solution, such as OH, H and OO, during the plasma treatments.

DOI： 10.1088/1361-6595/abbbd4

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Applied Surface Science  

The dependence of substrate temperatures (50 to −20 °C) on etch rate in two kinds of PECVD SiN films were investigated by a CF4/H2 mixture plasma. The XRR and XPS results indicate that the chemical composition and film density were almost identical for the films. The FTIR shows that the ratio of N[sbnd]H and Si[sbnd]H groups were found to be significantly different in the SiN films. The N[sbnd]H rich films exhibited a lower etch rate at −20 °C than that observed at room temperature or higher, whereas the Si[sbnd]H rich films showed a higher etch rate at −20 °C. We found that the fluorocarbon thickness was thicker in the Si[sbnd]H rich samples than N[sbnd]H rich samples. The fact suggests that hydrogen originated from the broken Si[sbnd]H bonds enhanced the polymerization, which causes the decrease of etch rate. A thinner fluorocarbon thickness was found in the Si[sbnd]H rich samples at low temperature, which results in the higher etch rate. Angular-resolved XPS indicates that N[sbnd]H bonding formed easier on film surface at −20 °C. These results indicate that the bonding structure and substrate temperature affected the fluorocarbon thickness, fluorine reaction probability and hydrogen dissociation during the SiN etching.

DOI： 10.1016/j.apsusc.2020.148550

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Applied Surface Science  

Gas chemistry has a significant impact on etch selectivity in semiconductor device fabrication, which is important for realization of atomic-scale removal and formation of high-aspect ratio features. To widen the controllable changes in the etchant composition in etching processes, our previous calculation showed the possibility of the controllable generation of CH2F and CHF2 related ions and radicals from a 1,1,2-trifluoroethane (CH2FCHF2) parent gas. The etch selectivity among silicon nitride (SiN), silicon dioxide (SiO2) and poly-Si films using CH2FCHF2 plasma mixed with O2 and Ar was investigated. The effects of the CH2FCHF2 and O2 partial pressures on the composition of CHF2+ and CH2F+ ions, which were measured with a quadrupole mass spectrometer, and on the possible reactions with respect to the CH2FCHF2 and O2 mixed gas phase were investigated using quantum chemical calculations. The etch selectivity was investigated through surface etching reactions for SiN, SiO2, and poly-Si films.

DOI： 10.1016/j.apsusc.2020.148439

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Japanese Journal of Applied Physics  

DOI： 10.35848/1347-4065/abd871

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Japanese Journal of Applied Physics  

Trypanosoma brucei (Tb) is a pathogenic protozoan causing sleeping sickness in humans. Despite little knowledge of how the produced reactive oxygen species (ROS) kills this protozoan, the research on the killing mechanism using chemical compounds and the phagosome in the macrophages has suggested that the protozoan is highly susceptible to the increased oxidative stress. Because the prescribed drug can react with various kinds of molecules and the second produced intermediate compounds, in this study, we clarified the immediate killing effect on Tb in the condition of increased oxidative stress using a low-temperature plasma at atmospheric pressure (LTP) equipment. Results Show the significant growth inhibition of Tb in the LTP-treated medium, the loss of morphological homeostasis with twisted to puffed appearance, and demonstrated the swelled changes on mitochondria and endoplasmic reticulum. In conclusion, this study revealed how the increased oxidative stress kills Tb using LTP technology.

DOI： 10.35848/1347-4065/abd464

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Nanomaterials  

Carbon nanowalls (CNWs), which are vertically oriented multi-layer graphene sheets, were employed in surface-assisted laser desorption/ionization mass spectrometry (SALDI-MS) measurements to detect low-molecular-weight organic compounds. CNWs substrates with widely different wall-to-wall distances from 142 to 467 nm were synthesized using a radical-injection plasma-enhanced chemical vapor deposition (RI-PECVD) system with nanosecond pulse biasing to a sample stage. When survival yield (SY) values of N-benzylpyridinium chloride (N-BP-Cl) were examined, which is commonly used to evaluate desorption/ionization efficiency, a narrower wall-to-wall distance presented a higher SY value. The highest SY value of 0.97 was realized at 4 mJ/cm2 for the highest-density CNWs with a wall-to-wall distance of 142 nm. The laser desorption/ionization effect of arginine, an amino acid, was also investigated. When CNWs with a narrower wall-to-wall distance were used, the signal-to-noise (SN) ratios of the arginine signals were increased, while the intensity ratios of fragment ions to arginine signals were suppressed. Therefore, the CNWs nanostructures are a powerful tool when used as a SALDI substrate for the highly efficient desorption/ionization of low-molecular-weight biomolecules.

DOI： 10.3390/nano11020262

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PubMed

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Scientific Reports  

The use of low-temperature plasma for the pre-sowing seed treatment is still in the early stage of research; thus, numerous factors affecting germination percentage, seedling growth, and yield remains unknown. This study aimed to estimate how two critical factors, such as harvest year and seed coat color, affect the percentage of germination and seedling growth after plasma treatment. Radish seeds stored for 2 and 1 year after harvesting (harvested in 2017 and 2018) were sorted into two colors (brown and grey) to investigate the plasma effect on harvest year and seed coat color. We analyzed the amounts of seed phytohormones and antioxidant (γ-tocopherol) were analyzed using mass spectrometry, and physical changes were studied using SEM, EDX, and EPR to understand the mechanism of plasma-induced changes in radish seeds. The obtained results revealed that plasma treatment on seeds affects the germination kinetics, and the maximal germination percentage depends on seed color and the time of seed storage after harvest. Through this study, for the first time, we demonstrated that physical and chemical changes in radish seeds after plasma treatment depends upon the seed color and harvest year. Positive effects of plasma treatment on growth are stronger for sprouts from seeds harvested in 2017 than in 2018. The plasma treatment effect on the sprouts germinated from grey seeds effect was stronger than sprouts from brown radish seeds. The amounts of gibberellin A3 and abscisic acid in control seeds strongly depended on the seed color, and plasma induced changes were better in grey seeds harvested in 2017. Therefore, this study reveals that Air scalar-DBD plasma's reactive oxygen and nitrogen species (RONS) can efficiently accelerate germination and growth in older seeds.

DOI： 10.1038/s41598-021-81175-x

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PubMed

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Japanese Journal of Applied Physics  

The ultraviolet photon-induced interface defects that degrade the performance of a semiconductor device are reduced by the optimal pulse repetition rate of a pulse-modulated inductively coupled plasma. The defect density depends on the pulse repetition rates; it takes minimum value at a few hundred pulses s−1 and peaks at a few k pulses s−1. The repetition rate-dependent behavior is suggested to be caused by the transient behavior between the plasma's ON and OFF phases. Note that controlling the transient behavior for reducing the photon-induced damage is essential.

DOI： 10.35848/1347-4065/abd113

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Plasma Processes and Polymers  

The application of cold plasma has attracted considerable attention in the field of agriculture. We examined the effects of plasma irradiation and treatment with plasma-activated Ringer's lactate solution (PAL) on rice seedlings in a paddy field. Irradiation during the vegetative growth period increased seedling growth, panicle number, and grain yield. In contrast, treatment during the reproductive growth period had a negative or no effect. Moreover, treatment with PAL solution promoted the growth of the main stem, such as grain number and panicle weight, and grain quality, but the grain yield from the whole plant was decreased. The results suggest that cold plasma treatment of rice seedlings is effective for improving plant growth, grain yield, and grain quality.

DOI： 10.1002/ppap.202000181

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Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Current Medicinal Chemistry  

Low-temperature plasma (LTP) is a partially ionized gas that contains elec-trons, ions, radicals, light, etc. Recently, the bio-medical application of LTP has become a hot topic in plasma science and biological science. Cancer treatment with plasma is the most challenging topic in plasma bio-medical applications. Many in vitro and in vivo ex-periments have been conducted to investigate the anti-tumor effects of LTP. Extracellular reactive oxygen and nitrogen species (RONS) in plasma-activated solutions are key factors for the anti-tumor effects, and amino acid modifications by LTP may affect cellular responses. Intracellular RONS are also key factors for the anti-tumor effects. Various signaling pathways, such as p53 signaling pathways, survival and proliferation signaling pathways, and oxidative stress-dependent signaling pathways are activated by LTP.

DOI： 10.2174/0929867328666210629121731

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PubMed

Language：English   Publishing type：Research paper (scientific journal)  

CiNii Research

Language：English   Publishing type：Research paper (scientific journal)  

CiNii Research

Language：English   Publishing type：Research paper (scientific journal)  

CiNii Research

Language：English   Publishing type：Research paper (scientific journal)  

CiNii Research

Language：English   Publishing type：Research paper (scientific journal)   Publisher：47th EPS Conference on Plasma Physics, EPS 2021  

Scopus

Language：English   Publishing type：Research paper (scientific journal)  

CiNii Research

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Carbon  

Controlling the layers and in-plane defects in multi-layer graphene is the key to exploiting the extraordinary properties of graphene. Layer-by-layer thinning under high-density oxygen neutrals was observed in situ during room-temperature reaction science using a remote oxygen plasma inside a high-voltage transmission electron microscopy. Even though the etching rate of graphene was higher at the edge than at the basal plane, etching started from both locations. Each etched layer was represented by the plasmon loss intensity in the electron energy loss spectrum. After exposure to the remote oxygen plasma, the electron diffraction pattern for the multi-layer graphene keep clear six-fold diffraction pattern. Raman spectroscopy revealed the formation of defects in multi-layer graphene. The nonthermal reaction of oxygen neutrals required for graphene etching was demonstrated by in situ transmission electron microscopy.

DOI： 10.1016/j.carbon.2020.07.052

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Journal of Crystal Growth  

III-nitride was grown by radical-enhanced metalorganic chemical vapor deposition (REMOCVD) with a very high-frequency electric source 100 MHz, using nitrogen and hydrogen as a source gas free from ammonia gas. Applying radio frequency (RF) power at the top electrode generates activated nitrogen, hydrogen, and other nitrogen species. Homoepitaxial gallium nitride (GaN) growth was studied as a function of chamber pressure by REMOCVD. The grown GaN was characterized by scanning electron microscope (SEM), atomic force microscope (AFM), and double crystal X-ray diffraction (XRD). Ga radicals and N radicals were detected by optical emission spectroscopy (OES) as a function of chamber pressure. The V/III ratio changes with the N2*/Ga* ratio, and the step flow growth of GaN was achieved under the chamber pressure of 300 Pa.

DOI： 10.1016/j.jcrysgro.2020.125863

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Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Journal of Physics D: Applied Physics  

The concept of using a glass substrate with fine through-holes filled with metal, called through-glass-vias (TGVs), for an inner wall of an enclosure of a nonequilibrium atmospheric pressure plasma source was validated to extend its processing area with high plasma densities maintained. When applying the TGV substrate into an inner wall of the plasma source, the generated discharge was less likely to drift along with the gas flow, which resembled the behavior of locally high electric fields of the plasma source, called the creeping mode. The decrease in breakdown voltage was also observed. These phenomena are caused by the TGV areas acting as a steering control material in the enclosure of the plasma source. The location of the TGV areas affected the behavior of the generated plasma. The shape of the plasma was accomplished to arbitrarily and locally control by the placement of TGVs.

DOI： 10.1088/1361-6463/aba1ad

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Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Scientific Reports  

A green method to synthesize spherical Sn particles by reducing SnO2 film in atmospheric-pressure H2/Ar plasma at low temperatures for various applications is presented. The floating wire-assisted remotely-generated plasma with a mixture of 0.05% H2/Ar gas formed spherical metallic Sn particles by reducing a SnO2 layer on glass substrate. During the reduction process, H radical density was measured by using vacuum ultraviolet absorption spectroscopy, and plasma properties including electron density and gas temperature were diagnosed by optical emission spectroscopy. The inductively coupled generated plasma with a high electron density of 1014 cm−3, a hydrogen atom density of 1014 cm−3, and a gas temperature of 940 K was obtained at a remote region distance of 150 mm where the SnO2/glass substrate was placed for plasma treatment. The process has been modeled on the spherical Sn formation based on the reduction of SnO2 films using H radicals. Depending on the treatment condition, the total reduction area, where spherical Sn particles formed, was enlarged and could reach 300 mm2 after 2 min. The substrate temperature affected the expansion rate of the total reduction area and the growth of the Sn spheres.

DOI： 10.1038/s41598-020-74663-z

Open Access

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PubMed

Language：English   Publishing type：Research paper (scientific journal)   Publisher：ACS Omega  

The growth of sputtered GaN at low temperature is strongly desired to realize the dissemination of low-cost GaN high electron mobility transistor devices for next-generation communication technology. In this work, the roles of atomic nitrogen (N)/hydrogen (H) in GaN film growth on AlN/sapphire substrates by chemically assisted dual source sputtering are studied at a low growth temperature of 600 °C under a pressure of 2 Pa using vacuum ultraviolet absorption spectroscopy. The lateral growth was strongly enhanced with an appropriate H/N flux ratio of 1.9 at a GaN growth rate of ∼1 μm h-1. X-ray photoelectron spectroscopy measurements indicated that N removal from the grown GaN surface by atomic hydrogen promoted the migration of Ga. A smooth GaN surface was achieved at a suitable N/Ga supply ratio of 53 and a H/N ratio of 1.9 with the addition of 0.5% chlorine to the Ar sputtering gas.

DOI： 10.1021/acsomega.0c03865

Open Access

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Scopus

PubMed

Language：English   Publishing type：Research paper (scientific journal)  

Web of Science

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Applied Physics Express  

Plasma-activated medium (PAM) is defined as a medium irradiated with non-thermal plasma; multiple in vitro and animal experiments have demonstrated that PAM exhibits anti-tumor effects against various cancers. PAM contains various reactive species that contribute to these anti-tumor effects. To increase the abundance of such reactive species, we used laser-generated plasma (LGP). We used a LGP consisting of 200 ns pulsed plasma with an electron density of approximately 7.0 × 1018 cm−3, which is an extremely high electron density, exceeding those of other atmospheric pressure plasmas. We created a laser-generated-plasma-activated medium (LPAM), and treated HeLa cells with the LPAM in both the presence and absence of catalase. Both with and without catalase, the LPAM treatment yielded strong anti-cancer effects against HeLa cells. Surprisingly, we observed morphological differences between HeLa cells grown in LPAM prepared with and without catalase. These results suggested that LPAM induces the cell death through extracellular hydrogen peroxide-dependent and -independent processes.

DOI： 10.35848/1882-0786/abb68c

Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Plasma Processes and Polymers  

We present a novel plasma system that can generate a plasma-activated medium by changing the proportion of reactive gases such as oxygen, nitrogen, and hydrogen in the plasma flow. The correlation between the biological activity of plasma-activated solutions prepared under multiple plasma gas-flow conditions was evaluated. Mixed nitrogen, in addition to oxygen, in the gas flow is most powerful for producing plasma-activated Ringer's lactate solution against antitumor effects on ovarian cancer cells as compared with oxygen or nitrogen alone. The antitumor effect of plasma-activated solutions is controllable by the modification of the proportion of reactive gases (especially nitrogen and oxygen gases) in the plasma flow. These results suggest that the plasma flow conditions may be one of the candidates for the specifications of the plasma-activated solutions to the therapeutic effect.

DOI： 10.1002/ppap.201900259

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Cell Death Discovery  

Gold nanoparticles (Au-NPs) have attracted attention as a promising sensitizer owing to their high atomic number (Z), and because they are considered fully multifunctional, they are preferred over other metal nanoparticles. Cold atmospheric plasma (CAP) has also recently gained attention, especially for cancer treatment, by inducing apoptosis through the formation of reactive oxygen species (ROS). In this study, the activity of different sized Au-NPs with helium-based CAP (He-CAP) was analyzed, and the underlying mechanism was investigated. Treating cells with only small Au-NPs (2 nm) significantly enhanced He-CAP-induced apoptosis. In comparison, 40 nm and 100 nm Au-NPs failed to enhance cell death. Mechanistically, the synergistic enhancement was due to 2 nm Au-NPs-induced decrease in intracellular glutathione, which led to the generation of intracellular ROS. He-CAP markedly induced ROS generation in an aqueous medium; however, treatment with He-CAP alone did not induce intracellular ROS formation. In contrast, the combined treatment significantly enhanced the intracellular formation of superoxide (O2• −) and hydroxyl radical (•OH). These findings indicate the potential therapeutic use of Au-NPs in combination with CAP and further clarify the role of Au-NPs in He-CAP-aided therapies.

DOI： 10.1038/s41420-020-00314-x

Open Access

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Scopus

PubMed

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Applied Physics Express  

He discharge in a coaxial dielectric barrier discharge (DBD) device develops in three stages: first, a Townsend-glow-type plasma spreads in the region between the electrodes; second, a plasma bullet (streamer type discharge) propagates axially and; third, the bullet transitions into a surface discharge at the dielectric surface. These mode transitions are quite different from planar type DBD, in which one discharge mode basically corresponds to one discharge pulse. From fluid-based numerical analysis, the bullet propagation is obeyed by trapping with strong electric fields induced by grounded electrode underneath the dielectric barrier and by surface charge accumulated on the dielectric surface.

DOI： 10.35848/1882-0786/aba3f2

Open Access

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Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Processes  

In recent years, non-thermal plasma (NTP) application in agriculture is rapidly increasing. Many published articles and reviews in the literature are focus on the post-harvest use of plasma in agriculture. However, the pre-harvest application of plasma still in its early stage. Therefore, in this review, we covered the effect of NTP and plasma-treated water (PTW) on seed germination and growth enhancement. Further, we will discuss the change in biochemical analysis, e.g., the variation in phytohormones, phytochemicals, and antioxidant levels of seeds after treatment with NTP and PTW. Lastly, we will address the possibility of using plasma in the actual agriculture field and prospects of this technology.

DOI： 10.3390/pr8081002

Open Access

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Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Archives of Biochemistry and Biophysics  

Ringer's lactate solution irradiated by non-thermal plasma, comprised of radicals, electrons, and ions, is defined as plasma-activated lactate (PAL). PAL exhibited antitumor effects in glioblastoma U251SP cells, which we termed PAL-specific regulated cell death. In contrast to the oxidative stress condition typical of cells incubated in plasma-activated medium (PAM), U251SP cells treated with Ringer's lactate solution or PAL exhibited changes in intracellular metabolites that were reductive in the redox state, as measured by the ratio of oxidative/reductive glutathione concentrations. In the metabolomic profiles of PAL-treated cells, the generation of acetyl-CoA increased for lipid metabolism from alanine and asparagine. PAL thus induces regulated death of U251SP glioblastoma cells in more innate microenvironments than PAM.

DOI： 10.1016/j.abb.2020.108414

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PubMed

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Journal of Vacuum Science and Technology A: Vacuum, Surfaces and Films  

Gallium nitride (GaN) semiconductor devices must be fabricated using plasma etching with precise control of the etching depths and minimal plasma-induced damage on the atomic scale. A cyclic process comprising etchant adsorption and product removal may be suitable for this purpose but an understanding of the associated etching surface reactions is required. The present work examined the formation of a chlorinated layer based on Cl radical adsorption on a GaN surface in conjunction with Ar ion irradiation. This research employed beam experiments and in situ x-ray photoelectron spectroscopy. The results show that N atoms are preferentially desorbed during exposure to Ar ions to produce Ga-rich layers at depths of 0.8 and 1.1 nm at an Ar ion dosage on the order of 1016 cm-2 and ion energies of 116.0 and 212.6 eV, respectively. Subsequent exposure of the irradiated Ga-rich layer to Cl radicals removes some Ga atoms and produces a chlorinated layer over the GaN surface. This chlorinated layer has a thickness on the order of 1 nm following Cl radical dosages on the order of 1019 cm-2. This study of plasma-treated surfaces is expected to assist in developing means of controlling the etching depth during the atomic layer etching of GaN via Ar ion bombardment.

DOI： 10.1116/6.0000124

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Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Journal of Physics D: Applied Physics  

When applying high-voltage direct current to a pin-to-plane electrode geometry with a distance of 2 mm under atmospheric pressure in argon gas, electrical breakdown forms primary then secondary streamers. The polarity of the applied voltage affects this streamer-propagating phenomenon. Properties such as propagation speed, streamer head size, and plasma generation are parameterized at nanosecond scales by computational simulations of a self-consistent, multi-species, multierature plasma fluid modeling approach. For positive polarity on the pin electrode, streamer-head propagation speeds up and streamer head size increases with increasing applied voltages. However, local electron density at the head decreases. For negative polarity, corona-like discharges form around the pin electrode under low applied voltages, and diffusive steamers form under high applied voltages. Secondary streamers re-propagate from the pin after primary streamer propagation, forming a plasma with a high electron density of 1021 m-3 for the positive polarity. We show that low-voltage operations with positive polarity are useful for stable high-electron-density discharges under atmospheric pressure argon.

DOI： 10.1088/1361-6463/ab7df0

Open Access

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Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Applied Physics Express  

In-plane modification of hexagonal boron nitride (hBN) is demonstrated via plasma in solution without acid/base addition. Electron spin resonance spectroscopy clearly reveals an increase in nitrogen vacancies in the hBN plane. This could be a simple route to functionalizing the two-dimensional surface of hBN. Simultaneously, hydroxylation occurs, accompanied by an increase in the zeta potential.

DOI： 10.35848/1882-0786/ab916c

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Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Plasma Science and Technology  

A non-equilibrium atmospheric pressure argon (Ar) plasma excited by microsecond pulse is studied experimentally by laser scattering and optical emission spectroscopy (OES), and theoretically by collisional-radiative (CR) model. More specifically, the electron temperature and electron density of plasma are obtained directly by the laser Thomson scattering, the gas temperature is measured by laser Raman scattering, the optical emissions of excited Ar states of plasma are measured by OES. The laser scattering results show that the electron temperature is about 1 eV which is similar to that excited by 60 Hz AC power, but the gas temperature is as low as 300 K compared to about 700 K excited by 60 Hz AC power. It is shown that the microsecond pulsed power supply, rather than nanosecond ones, is short enough to reduce the gas temperature of atmospheric pressure plasma to near room temperature. The electron temperature and electron density are also obtained by CR model based on OES, and find that the intensities of the optical emission intensity lines of 727.41, 811.73, 841.08, 842.83, 852.44 and 912.86 nm of Ar can be used to characterize the behavior of electron density and electron temperature, it is very useful to quickly estimate the activity of the atmospheric pressure Ar plasma in many applications.

DOI： 10.1088/2058-6272/ab84e2

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Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Japanese Journal of Applied Physics  

We investigated fluoromethane compounds (CF4, CF3, CHF3, CH2F2, and CH3F) to examine their electronic properties and primary dissociation channels by using computational chemistry. For the electron attachment process, it was very important to represent the observed negative mass spectrum as a function of electron energy that calculation by the MP2 method for the negative ion and subsequent calculation by the EOMCCSD method were used to more accurately estimate the ground and the first excited states of the negative ion. In the evaluation of dissociation channels through the excitation process, the structure change of the excited fragment (from pyramidal to planar) was taken into account. Evaluation of Jahn-Teller distortion for the highly symmetrical CHF3 and CH3F was also very important to estimate the fragmentation process through the excitation. The calculated results after these treatments gave satisfactory representation of the experimental values. Moreover some predictions of experimentally unknown values are proposed.

DOI： 10.35848/1347-4065/ab7e3f

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Trends in Food Science and Technology  

Background: Nowadays, electron spin resonance (ESR) is widely used as a powerful, non-destructive and very sensitive technique for the detection of free radicals in food systems. It can be applied for the direct identification of highly reactive oxygen species, organic and inorganic paramagnetic species and screening of food for potential toxicity. Its applications cover investigating food oxidative stability and properties of irradiated foods including fruits and vegetables, meats and fishes, spices, cereal grains, and oil seeds. Scope and approach: This review aims at providing specialists in food science and industry with the fundamentals of ESR spectroscopy, typical radicals present in foods and their sources, ESR modalities, and detailed account for the use of the technology for evaluation of the physicochemical and nutritional properties of foods. Examples illustrating ESR applications for the evaluation of the effects of innovative and emerging technologies (ionizing radiation, high pressures, pulsed electric fields, cold plasma and ultrasonication) are discussed. Key findings and conclusions: ESR can be used for the identification/quantification of free radicals in foods, for spin-label oximetry, estimation of free radical scavenging, food stability, and chelating activity, with particular interest for food processed using innovative technologies, with the main advantages of its high sensitivity, specificity, and low amounts of sample needed and nowadays many types of ESR instruments are commercially available. However, due to the different nature of foods, the development of novel ESR techniques and methods of analysis specially designed to study foods is of great interest in the future.

DOI： 10.1016/j.tifs.2020.03.032

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Japanese Journal of Applied Physics  

DOI： 10.35848/1347-4065/ab8acf

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Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Carbon  

Carbon nanowalls (CNWs) are vertically standing, interconnecting flake- or wall-like collections of graphene sheets. In the present work, this material was synthesized by applying precisely controlled high-voltage nanosecond pulses to a substrate using an inductor energy storage circuit in a radical-injection plasma-enhanced chemical vapor deposition system, employing a CH4/H2 plasma. The resulting interconnected networks had a low density of CNWs with large average wall-to-wall distances. During the application of short-period pulses, the entire substrate surface was uniformly activated, thus enhancing the adsorption of carbon precursors and preventing CNW nucleation. As a result, an amorphous carbon film covered the surface of the substrate and a low CNW density was obtained with average wall-to-wall distances greater than 700 nm. On the basis of these results, the growth mechanism of CNWs was modeled.

DOI： 10.1016/j.carbon.2020.01.064

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Diamond and Related Materials  

Hydrogenated amorphous carbon (a-C:H) films comprise nanoclustering graphites (nc-G), fused aromatic rings (nR), and olefinic chain clusters (nC) of sp2-bonded carbons in an sp3 matrix. In this study, the sp2 composition of the nc-G, nR and nC in a-C:H films is found to be determined by the ion bombardment energy flux (ΓEi), which can be estimated as the product of ion bombardment energy and ion flux onto the deposited surface, in plasma-enhanced chemical vapor deposition using a plasma mixture of H2 and CH4 gases with the H radical injection method. The sp2 composition is analyzed using Raman spectroscopy and near-edge X-ray absorption structure spectroscopy. a-C:H becomes increasingly graphitized with increasing ΓEi. The precise control of the sp2 C structure composition can be achieved by controlling the very-high-frequency input power and radio frequency input bias power via the ion flux and ion bombardment energy.

DOI： 10.1016/j.diamond.2019.107651

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：ChemNanoMat  

Nanometer-size graphene sheets (nanographene) were synthesized by the in-liquid plasma method employing a mixture of alcohols. Pure methanol in-liquid plasma was found to not synthesize any nanographene. Pure ethanol synthesized nanographene with high crystallinity. Highly crystalline nanographene with a narrow full width-half maximum of the Raman scattering G-band (FWHMG) was obtained by mixing 1-butanol with methanol. This is due to the formation of carbon ring structures being inhibited by the addition of methanol. The ratio of added methanol determined the nanographene crystallinity and yield under a trade-off relationship, allowing the crystallinity and nanographene yield to be controlled by controlling the ratio. Gas chromatography-mass spectrometric analysis of by-products in the liquids’ supernatant showed that the crystallinity of the synthesized nanographene correlated with the ratio of carbon over oxygen of the alcohol precursors (C/O), i. e., the amount of hydroxyl groups in the liquids, and hence controlling the C/O ratio can be used to control the graphene crystallinity in the in-liquid plasma synthesis.

DOI： 10.1002/cnma.201900676

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Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Journal of Applied Physics  

In this work, first principles calculations combined with advanced surface diagnostics are used to unravel the mechanisms of plasma oxygen interaction with organic films of interest for advanced patterning in semiconductor device manufacturing. Results from a combination of x-ray photoelectron spectroscopy (XPS) diagnosed oxygen plasma exposed polystyrene films and first principles modeling of organic films (polystyrene, polyethylene, and derivatives) provide insights into how organic films are oxidized by oxygen atoms. XPS measurements show the rapid formation of C-O structures and their saturation after oxygen exposure on both pristine and argon bombarded polystyrene samples. Quantum mechanics calculations confirm that C-OH formation can be immediate without recourse to previously formed dangling bonds. Multiple oxygen impacts are required for scission of pristine ethylene carbon strands. Therefore, ethylene films can be converted to polyols that are stable, whereas more likely strands are broken before polyol formation through the formation of water and C=O. On the contrary, intermediate compounds with adjacent C=O bonds are not likely to form stable structures. The combination of XPS measurements and modeling implies that the oxidation of polystyrene and polyethylene is self-limiting on both hydrogen saturated and dehydrogenated (after argon ion plasma bombardment) surfaces.

DOI： 10.1063/1.5127863

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Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Japanese Journal of Applied Physics  

A brief history of the development of our plasma technology for the disinfection of agricultural harvests is presented in this review. We focused on the influence of reactive oxygen species (ROS), e.g. ground-state oxygen atoms [O(3P j )], excited-state oxygen molecules [O2(1Δg)], and ozone (O3), generated from atmospheric-pressure plasmas on the inactivation of fungal spores under dry conditions. For elucidating the inactivation mechanisms, it is essential to reveal the key ROS. Using some powerful tools, we revealed that the dose of O(3P j ) strongly correlates with the inactivation of fungal spores when compared to those of another ROS, such as O2(1Δg) and O3. The balance of antioxidants in the spores is possibly modulated by O(3P j ), leading to oxidation of organelles in spores. Herein, we introduce and discuss how O(3P j ) contributes to the inactivation of fungal spores associated with in situ diagnostics of plasma generated ROS and in situ intracellular observations of a few fungal spore species.

DOI： 10.35848/1347-4065/abcbd1

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Japanese Journal of Applied Physics  

Characterizing the interactions between plasma and living organisms has become a multidisciplinary topic in the field of low-temperature plasma science and technology. Living organisms are hierarchically comprised of cells, tissues, organs, and organ systems. Adaptive responses are systematically controlled by the state of the surrounding environment, such as when living organisms are irradiated with discharge plasma. This review is written from a biological perspective and focuses on the importance of gas temperature control in nonequilibrium atmospheric pressure plasmas. We discuss the critical parameters associated with direct plasma treatments of living organisms. This review provides an assessment of the status of this research field and addresses the prospects for further developments in understanding the interactions between plasma and living organisms. We address the importance and necessity of normothermic plasma treatment, where an experimental system involving living organisms is controlled at an optimal temperature, which plays a significant role in plasma biology.

DOI： 10.35848/1347-4065/abcbd2

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：21st International Conference on Miniaturized Systems for Chemistry and Life Sciences, MicroTAS 2017  

We present a study of blood microfiltration system towards optimal approach of non-invasive liquid biopsy for cancer detection by circulating tumor cells (CTCs). Filtration behavior of a microfilter was experimentally analyzed for tumor cell isolation from leukocytes in whole blood. This approach achieved an average of >96% recovery of spiked tumor cells and >99% total leukocytes depletion.

Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：21st International Conference on Miniaturized Systems for Chemistry and Life Sciences, MicroTAS 2017  

We developed a microfluidic chip for depositing single cells in microwells using simple micropipette operation. Cells were delivered to microwells by the meniscus motion of liquid interface. The residue deposits of cells were redistributed with air injection, and the isolated single cells were stored in microwells. Different microwell sizes and depths were studied to evaluate the trapping possibility of cells. Medium replacement and cell viability staining with the isolated single cells were achieved in microwells.

Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：IEEE International Symposium on Semiconductor Manufacturing Conference Proceedings  

The dependences of plasmas (CF4/D2 and CF4/H2) on etch rates of the PECVD SiN films at different substrate temperatures were investigated. The CF4/D2 plasma exhibited higher etch rates than that for the CF4/D2 plasma at room temperature and higher. The optical emission spectra showed that the CF polymerization, F and Balmer emissions were stronger in the CF4/D2 plasma, by comparing with the CF4/H2 plasma. A thinner fluorocarbon thickness with a lower F/C ratio was found in the sample proceeded by the CF4/H2 plasma. The fluorocarbon thickness and gas phase concentration were not responsible for the increase of etch rate in the CF4/D2 plasma. The abstraction of H inside the SiN films by deuterium and hydrogen dissociation were considered to be important for the etching of the Si-H bond rich SiN films.

DOI： 10.1109/ISSM51728.2020.9377537

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Journal of Physics D: Applied Physics  

Isotropic atomic-layer etching (ALE) of TiN-by using a plasma-assisted thermal-cyclic process with a 300-mm tool-was demonstrated. The process consists of exposure to a downstream CHF3/O2 plasma (for surface modification) followed by infrared irradiation for thermal desorption of the modified surface. Etched amount of TiN per cycle saturated at around 0.6 nm/cycle with respect to both radical-exposure time and infrared-irradiation time. To examine the reaction mechanism of the cyclic etching, the surfaces of TiN samples after CHF3/O2 plasma exposure were analyzed by in situ X-ray photoelectron spectroscopy (XPS). Self-limiting formation of the surface-modified layer, which was tentatively identified as an ammonium salt such as (NH4)xTiFy, was observed after radical exposure. It was confirmed by in situ XPS that the surface-modified layer was removed after thermal annealing at 110 °C. Isotropic ALE of TiN was thus demonstrated by using formation and desorption of ammonium salt in CHF3/O2 downstream plasma, which was also used for isotropic ALE of Si3N4.

DOI： 10.1088/1361-6463/ab3cf3

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Journal of Vacuum Science and Technology B: Nanotechnology and Microelectronics  

Nitrogen atoms are versatile for nitridation applications and do not lead to plasma-induced damage. Large-sized wafer processing demands a uniform supply of nitrogen atoms produced in a high-density very-high-frequency excited plasma of N2 without ammonia. The confinement of plasma through the use of a plasma shield plate (PSP) allows the samples to be separated in a downstream chamber. Generation and transport of N atoms were computationally simulated, and the PSP designs were implemented by PSP parameterization. The supply of high-density N radicals to the sample stage was optimally designed with sufficiently small holes and thin PSP to satisfy an aspect ratio of thickness-to-hole-diameter of less than 2.5.

DOI： 10.1116/1.5114831

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1038/s41598-019-50136-w

Open Access

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PubMed

Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.3390/c5030040

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Journal of Vacuum Science and Technology A: Vacuum, Surfaces and Films  

Self-limiting reactions of ammonium salt in CHF3/O2 downstream plasma were demonstrated for thermal-cyclic atomic layer etching (ALE) of Si3N4. In situ x-ray photoelectron spectroscopy analysis shows that an (NH4)2SiF6 by-product of the same thickness forms on Si3N4 in a wide gas composition range. The (NH4)2SiF6 layer prevents etching of Si3N4 during continuous plasma exposure in that wide range. The (NH4)2SiF6 layer was sublimated by heating, which was consistent with the result of the thermodynamic calculation. The reactions of the (NH4)2SiF6 layer in CHF3/O2 downstream plasma are used for thermal-cyclic ALE of Si3N4 with a newly developed 300-mm tool equipped with an in situ ellipsometer. It was confirmed that the amount etched per cycle saturates with respect to both plasma exposure time and infrared irradiation time.

DOI： 10.1116/1.5111663

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Plasma Processes and Polymers  

The developments in advanced interconnect technology for semiconductor logic devices for the mitigation of plasma-induced damage to low-dielectric-constant (low-k) materials, including fluorosilicate glass and carbon-doped silicon oxide is reviewed. The chemical bond structures of low-k materials are summarized to help mitigate the k value degradation caused by moisture uptake after plasma processes. Damage suppression is accomplished by integrating deposition chemistries, pattern etch transfer, and post-etch cleaning technologies. On the basis of analyses results, a discussion on the bond engineering of low-k materials and their degradation during plasma processing is given. Challenges facing low-k interconnect technology are also addressed.

DOI： 10.1002/ppap.201900039

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Plasma Processes and Polymers  

This study assesses a potential use of the recently developed nonthermal atmospheric pressure plasma technology in hydroponic plant cultivation. Two types of plasma-activated liquid solutions were compared, namely, l-Phenylalanine (l-Phe), which had a benzene ring structure, and l-Alanine (l-Ala), which did not have a benzene ring structure. Antimicrobial property and plant growth enhancement were simultaneously obtained when plasma-activated l-Phe was used. We found that the benzene ring structure in solution contributed to antimicrobial property. Further, colony forming unit assay indicated that 99% of Escherichia coli (E. coli) were eliminated after 24-h incubation and radish sprout growth increased by about 40% after 2 days of cultivation.

DOI： 10.1002/ppap.201900023

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Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：ACS Applied Bio Materials  

Nanostructured cell-culture scaffolds of carbon nanowalls (CNWs) were prepared by changing average wall-to-wall distances either 132 or 220 nm. Osteoblast-like cells (Saos-2) proliferated during 4 day incubation on the wider (220 nm) CNW scaffolds in the presence of electrical stimulation (ES). Differentiation gene expression levels of Runt-related transcription factor 2 (Runx2) and osteocalcin (OC) were suppressed after 10 day incubation, which indicated that the average wall-to-wall distances of the CNW scaffolds affect suppression of Runx2 and OC gene expression. This technique holds promise for controlling the differentiation of osteoblast-like cells.

DOI： 10.1021/acsabm.9b00178

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PubMed

Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.7567/1347-4065/ab163e

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.7567/1882-0786/ab1a58

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.7567/1347-4065/ab163a

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.7567/1347-4065/ab163b

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.7567/1347-4065/ab1638

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Japanese Journal of Applied Physics  

Electronic properties of fluoroethane compounds except C2H5F, C2H4F2, CH3CF3, C2H2F4, and C2F6 have not been reported. On the other hands, the physicochemical properties were reported for the usage as the alternative refrigerants. Dissociation channels in the process plasma for fluoroethane compounds were not fully discussed except 1,1,1,2-C2H2F4. Therefore we have investigated the electronic properties and primarily dissociation channels of fluoroethane compounds in the process plasma in semiconductor manufacturing, using computational chemistry. Positive and negative ionized states were investigated by density functional method and the excited states were investigated by EOMCCSD/aug-cc-pVDZ and TD-SCF CAM-B3LYP/aug-cc-pVDZ. It was generally shown through these investigations that C-C bond scission occurred by excitation and ionization and C-F bond scission occurred by excitation and electron attachment.

DOI： 10.7567/1347-4065/ab09ca

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Scopus

Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1002/ppap.201800175

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Journal of Materials Science: Materials in Electronics  

A three-dimensional (3D) glass integrated passive device (IPD) is an evolutionally advanced configuration to dramatically reduce the electronics form factor and manufacturing cost of current IPDs by introducing ultra-thin glass with through-glass-vias (TGVs). A defect-free TGV formation technology in polymer-laminated glass substrates is required to realize a highly reliable 3D glass IPD. This paper discusses mechanisms of each defect formation in the use of several types of lasers to explore suitable technology for defect-free drilling in polymer-laminated glass.

DOI： 10.1007/s10854-019-01354-5

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Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Micro and Nano Engineering  

The chemical bonding structure of porous low-k carbon-doped silicon oxide (SiOC) films (k < 2.4) was engineered using plasma-enhanced chemical vapor deposition and electron-beam curing. The high carbon concentration in the SiOC films with di-methyl bonds ([dbnd]Si(–]CH3)2) is crucial for resistance to plasma-induced damage (PID) and prevention of moisture uptake after the plasma treatment. The mix of di-methyl bonds is believed to be the key to protecting the films from PID because the films retain their hydrophobic characteristics even after plasma treatment. Thus, control of the ratio of di-methyl bonds to mono-methyl bonds ([tbnd]Si–]CH3) in the as-deposited SiOC film is necessary. Selection of trimethyl silane as a precursor for film matrix formation resulted in excellent control of this ratio to obtain highly reliable low-k/Cu interconnects for high-performance logic devices.

DOI： 10.1016/j.mne.2019.02.005

Open Access

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Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Journal of Vacuum Science and Technology B: Nanotechnology and Microelectronics  

Epitaxial growth of GaN films at a low temperature of 800 °C was studied in radical-enhanced metal-organic chemical vapor deposition, focusing on the discharge region of the plasma of a mixture of N2 and H2 gases. The effect of plasma confinement on the growth is crucial for realizing high crystal quality of grown GaN films, owing to the suppression of plasma-induced damage and decomposition of gallium precursors in the gaseous phase. By confined plasma in the discharge region using the plasma shield plates made of metal with multiple small holes effectively, GaN with a relatively flat surface was grown under conditions of higher V/III ratios. Epitaxial growth of GaN films was achieved by modifying the plate design and controlling the high V/III ratio using both the plasma-excitation power and the Ga precursor flow rate.

DOI： 10.1116/1.5083970

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Micro and Nano Engineering  

The publisher regrets that we missed to publish the conflict of interest statement in the original article. The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper. The publisher would like to apologise for any inconvenience caused.

DOI： 10.1016/j.mne.2019.05.004

Open Access

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Scopus

Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1088/1361-6463/ab03c4

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1088/1361-6463/aaff44

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1109/TBCAS.2018.2882472

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PubMed

Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1088/1361-6463/aaf8e0

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Japanese Journal of Applied Physics  

Amorphous carbon (a-C) thin films were deposited under the control of C2 radical density using radical-injection plasma-enhanced chemical vapor deposition (RI-PECVD) with CH4/H2 plasma. By actinometric monitoring of C2 emission intensities, the plasma parameters were precisely controlled by changing in CH4-containing plasma excitation power independent of H2 plasma excitation. The control of the incorporation of sp2-C clusters in the a-C films during the a-C film depositions is demonstrated by tailoring Raman positions vs. full widths at half maxima for the G band around 1580 cm-1 to the RI-PECVD parameters.

DOI： 10.7567/1347-4065/aafd49

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1116/1.5082345

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.3390/c5010008

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DOI： 10.3390/c5010007

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DOI： 10.1016/j.abb.2018.12.001

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PubMed

Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1063/1.5081875

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1088/1361-6463/aaf460

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.7567/1882-0786/aaf469

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.7567/1347-4065/aafb5b

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.7567/1347-4065/aaf92a

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.7567/1347-4065/aaeb39

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.7567/1347-4065/aaec87

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：ACS Applied Nano Materials  

The in situ binding of tin oxide (SnO2) nanoparticles (SNp) and graphene nanosheets (GNs) that synthesized simultaneously in single-step atmospheric-pressure processing was achieved at a low temperature by employing in-liquid plasma in a solution of tin chloride (SnCl2·2H2O) in ethanol as the only precursor. Transmission electron microscopy, Raman analysis, and X-ray diffraction revealed the composite (SNp/GNs) synthesis with SNp of sizes 2-3 nm, which were distributed uniformly and attached to both sides of the GNs. The SNp/GNs composite synthesis was provided by the simple, low-cost, single-processing method of the in-liquid plasma for future gas-sensing and lithium-ion battery applications.

DOI： 10.1021/acsanm.8b02201

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.7567/1882-0786/aaf0ab

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：The Institute of Electrical Engineers of Japan  

<p>A nano-gap electrode array is batch-fabricated based on photolithography. A high resolution is obtained by using an over-hanging resist cover on the under-etched metal film. The process includes two-time mask-patterning. The first photoresist is UV-cured, allowing second patterning without degrading the first pattern. A nano-gap width of 237±63 nm is obtained from a 704-electrode array with an yield of 97%.</p>

DOI： 10.1541/ieejsmas.139.27

CiNii Research

Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1515/hsz-2018-0199

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PubMed

Language：English   Publishing type：Research paper (scientific journal)   Publisher：23rd International Conference on Miniaturized Systems for Chemistry and Life Sciences, MicroTAS 2019  

We present a study of microbial Raman spectroscopy towards optimal approach of rapid microbiological methods (RMMs). Raman spectra of single microorganism cells were measured and analyzed by data clustering to identify the microbial species without culturing for colony formation.

Scopus

Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1063/1.5050819

Open Access

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.7567/JJAP.57.106502

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1016/j.vacuum.2018.07.040

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1088/1361-6463/aad510

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：IEEE International Symposium on Semiconductor Manufacturing Conference Proceedings  

Our developed non-contact method for measurement of temperature of silicon (Si) wafer by using autocorrelation-type fourier domain low coherence interferometer has advantageous in accuracy and rapid response. We demonstrate measurements in temperature for Si wafer at real-time during plasma process and in estimation of heat flux to the wafer from plasma, involving heats balanced plasma source and conductive loss in Si. The analysis indicated that other heat sources like the chamber parts with relatively high temperature impact on the duty ratio during the process with feedback control of the wafer teperture.

DOI： 10.1109/ISSM.2018.8651183

Scopus

Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.7567/JJAP.57.06JC02

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.7567/JJAP.57.06JD01

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.7567/JJAP.57.06JA01

Open Access

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.7567/JJAP.57.06JF03

Open Access

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.7567/JJAP.57.06JF01

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.7567/JJAP.57.06JE03

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.7567/JJAP.57.06J001

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.7567/JJAP.57.045101

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.7567/JJAP.57.040303

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1088/1361-6463/aaab09

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1088/1361-6463/aaa885

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.7567/JJAP.57.037001

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1002/ppap.201700200

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.7567/JJAP.57.026201

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.7567/JJAP.57.01A001

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.7567/JJAP.57.0102B4

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.7567/APEX.11.015102

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1111/pin.12617

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PubMed

Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1088/1361-6595/aaa22e

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1177/2155179017733152

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PubMed

Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1117/12.2297241

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1109/trpms.2017.2721973

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：22nd International Conference on Miniaturized Systems for Chemistry and Life Sciences, MicroTAS 2018  

We present a study of genomic profiling for circulating tumor cells (CTCs) using a blood microfiltration system. DNA amplification of CTCs was performed with a microfilter for single cancer cells in a clinical setting. This strategy was successfully used to detect the driver mutations in epidermal growth factor (EGF) receptor oncogenes by quantitative PCR and characterize the dosing effect of molecularly targeted drug for lung cancer.

Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：22nd International Conference on Miniaturized Systems for Chemistry and Life Sciences, MicroTAS 2018  

We present a study of centrifugal filtration device toward easy-to-use approach of non-invasive liquid biopsy for cancer diagnosis by cell-derived nanoscale vesicles (exosomes). A phase-dispersed glass filter having nanoporous structure was embedded into a spin column to trap exosomes with small centrifuge. This device enabled over 90% exosome isolation from biological samples within 10 minutes.

Scopus

Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1063/1.4999256

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.7567/JJAP.56.126503

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Reviews of Modern Plasma Physics  

Plasma medical science is a novel interdisciplinary field that combines studies on plasma science and medical science, with the anticipation that understanding the scientific principles governing plasma medical science will lead to innovations in the field. Non-thermal atmospheric pressure plasma has been used for medical treatments, such as for cancer, blood coagulation, and wound healing. The interactions that occur between plasma and cells/tissues have been analyzed extensively. Direct and indirect treatment of cells with plasma has broadened the applications of non-thermal atmospheric pressure plasma in medicine. Examples of indirect treatment include plasma-assisted immune-therapy and plasma-activated medium. Controlling intracellular redox balance may be key in plasma cancer treatment. Animal studies are required to test the effectiveness and safety of these treatments for future clinical applications.

DOI： 10.1007/s41614-017-0004-3

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1002/ppap.201700123

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1116/1.4994218

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1063/1.5006598

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1088/1361-6463/aa8131

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1038/s41598-017-11877-8

Open Access

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PubMed

Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1116/1.4997170

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PubMed

Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.7567/APEX.10.086502

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.7567/JJAP.56.076202

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1039/c7cp00489c

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PubMed

Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.7567/JJAP.56.06H001

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.7567/JJAP.56.06HA02

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.7567/JJAP.56.06HF03

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.7567/JJAP.56.06HE08

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.7567/JJAP.56.06HC03

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1088/1361-6463/aa6874

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1088/1361-6463/aa6555

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1088/1361-6463/aa61d7

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1088/1361-6463/aa5f1d

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1088/1361-6463/aa60f7

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.7567/APEX.10.036201

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.7567/JJAP.56.035101

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.7567/JJAP.56.026502

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1063/1.4974821

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Japanese Journal of Applied Physics  

Deep ultraviolet (UV) photons emitted from Cl2 plasmas become a critical cause of degradation in both photoluminescence (PL) properties and surface stoichiometry as a result of plasma-induced damage on GaN films in Cl2 plasma etching at high temperatures. The damages were formed thermally by photon-irradiations of plasma UV emissions with wavelengths of >258-306 nm from Cl2 plasma at temperatures greater than 500 °C. The damage were observed with a depth of approximately 3.2 nm. The PL property degraded by the UV emission-induced damage at an early period of plasma etching and reached a constant value.

DOI： 10.7567/JJAP.56.096501

Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：ECS Transactions  

A highly selective, rapid thermal-cyclic atomic-level etching (ALE) process for SiNx films has been developed. The first step of this process is exposing SiNx to hydrofluorocarbon plasma to form an (NH4)2SiF6 layer on the SiNx surface. The second step is rapid thermal annealing with infrared (IR) irradiation to decompose and sublimate the (NH4)2SiF6 layer. Etching of SiNx was observed after the (NH4)2SiF6 layer was removed by thermal annealing. Cyclic etching tests were carried out by repeated plasma exposure and IR irradiation. It was found that the cyclic process is self-limiting because etching depth depends only on the cycle number and not on the plasma exposure time. A high selectivity over SiC2 and poly Si was confirmed. This paper reviews the novel isotropic ALE for nitride films focusing on the surface reaction mechanism investigated by x-ray photoelectron spectroscopy (XPS) and thermal desorption spectroscopy (TDS). Isotropic ALE of TiN was also demonstrated using the same approach.

DOI： 10.1149/08003.0003ecst

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Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1116/1.4949570

Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.3892/ijmm.2016.2574

Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1016/j.abb.2016.03.023

Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.7567/APEX.7.046201

Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1002/ppap.201500229

Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1016/j.abb.2016.01.011

Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1002/ppap.201570043

Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1002/ppap.201500132

Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.7567/JJAP.55.01AB04

Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)  

Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1002/ppap.201500099

Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1016/j.cpme.2015.09.001

Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1371/journal.pone.0136956

Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1109/TSM.2015.2470554

Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)  

Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.7567/JJAP.54.06GB04

Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.7567/JJAP.54.06GA03

Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.7567/JJAP.55.040305

Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.7567/JJAP.54.040303

Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1088/0963-0252/24/2/025019

Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.7567/JJAP.54.040301

Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1016/j.tsf.2014.10.021

Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1016/j.tsf.2014.10.020

Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1063/1.4905901

Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1088/0022-3727/48/4/045202

Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1109/TPS.2014.2353659

Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.7567/JJAP.54.01AG05

Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.7567/JJAP.54.01AB03

Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1063/1.4896833

Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1088/0022-3727/47/42/422002