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DOI： 10.1039/d3cc02986g

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Publishing type：Research paper (scientific journal)   Publisher：American Physical Society (APS)  

DOI： 10.1103/PhysRevB.107.155123

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Other Link： http://harvest.aps.org/v2/journals/articles/10.1103/PhysRevB.107.155123/fulltext

Language：English   Publishing type：Research paper (scientific journal)   Publisher：American Chemical Society (ACS)  

DOI： 10.1021/acsmaterialsau.2c00081

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DOI： 10.35848/1882-0786/acbbb8

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：The Chemical Society of Japan  

<p>We report carbon nanotube (CNT) gels, formed by mechanically mixing CNTs, organic solvents, and a small molecule, Trip-Phz, that have a strong affinity for fullerene materials. There is a clear threshold value in the amount of Trip-Phz needed for the transition from soft to hard gels.</p>

DOI： 10.1246/cl.220319

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry (RSC)  

Nitrogen-doped nonalternant aromatic belt was synthesized via palladium-catalyzed six-fold annulative double N-arylation reaction. The highly symmetric structure and multistep oxidation behavior of the N-belt were confirmed.

DOI： 10.1039/d2sc02647c

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：American Chemical Society (ACS)  

DOI： 10.1021/acsami.2c09302

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This study describes the concise exfoliation of multilayer Ti3C2T x MXene containing residual aluminum atoms. Treatment with tetramethylammonium base in a co-solvent of tetrahydrofuran and H2O produced single-layer Ti3C2T x , which was confirmed via atomic force microscopy observations, with an electrical conductivity 100+ times that of Ti3C2T x prepared under previously reported conditions. The scanning electron microscopy and X-ray diffraction measurements showed that the exfoliated single-layer Ti3C2T x MXenes were reconstructed to assembled large-domain layered films, enabling excellent macroscale electric conductivity. X-ray photoelectron spectroscopy confirmed the complete removal of residual Al atoms and the replacement of surface fluorine atoms with hydroxy groups. Using the exfoliated dispersion, a flexible transparent conductive film was formed and demonstrated in an electrical application.

DOI： 10.3389/fchem.2022.841313

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

DOI： 10.1039/d1tc05161j

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Language：Japanese   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry (RSC)  

<p>Supramolecular chiral crystals of radical anion salts of a triangular chiral electron acceptor, (−)-naphthalene diimide (NDI)-Δ, were electrochemically grown in propylene carbonate electrolyte solutions in the presence of cyclic multidentate ligands.</p>

DOI： 10.1039/d1ce00628b

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：American Chemical Society ({ACS})  

DOI： 10.1021/acsami.1c08417

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

DOI： 10.1016/j.apsusc.2020.148642

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：American Chemical Society (ACS)  

DOI： 10.1021/acs.cgd.0c01176

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

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Authorship：Lead author   Language：Japanese   Publishing type：Research paper (scientific journal)   Publisher：Japan Society for Molecular Science  

<p>In the graph theory, it is known that the line graphs of the <i>K</i>₄ and diamond lattices are the hyper-kagome and pyrochlore lattices, respectively. The hyper-kagome and pyrochlore lattices are possible frustration lattices, because they consist of a triangular or tetrahedral component. In the present article, we describe the crystal structures and physical properties of a molecule-based <i>K</i>₄, (–)-NDI-Δ, and a molecule-based diamond, bpBDTDA. The line graph transformation reveals a spin frustration in (–)-NDI-Δ, which results in a spin liquid ground state, and a bond frustrations in bpBDTDA, which induces a stepwise and inhomogeneous lattice dimerization.</p>

DOI： 10.3175/molsci.14.a0113

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：NATURE PUBLISHING GROUP  

Scanning tunneling microscopy (STM) observation reveals that a cyclic thiazyl diradical, BDTDA (=4,4'-bis(1,2,3,5-dithiadiazolyl)), forms a well-ordered monolayer honeycomb lattice consisting of paramagnetic corners with unpaired electrons on a clean Cu(111) surface. This BDTDA lattice is commensurate with the triangular lattice of Cu(111), with the former being 3 x 3 larger than the latter. The formation of the BDTDA monolayer structure, which is significantly different from its bulk form, is attributed to an interaction with the metal surface as well as the intermolecular assembling forces. STM spectroscopy measurements on the BDTDA molecules indicate the presence of a characteristic zero-bias anomaly centered at the Fermi energy. The origin of this zero-bias anomaly is discussed in terms of the Dirac cones inherent to the honeycomb structure.

DOI： 10.1038/srep18359

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：AMER CHEMICAL SOC  

The K-4 structure was theoretically predicted for trivalent chemical species, such as sp(2) carbon. However, since attempts to synthesize the K-4 carbon have not succeeded, this allotrope has been regarded as a crystal form that might not exist in nature. In the present work, we carried out electrochemical crystallization of the radical anion salts of a triangular molecule, naphthalene diimide (NDI)-Delta, using various electrolytes. X-ray crystal analysis of the obtained crystals revealed the K-4 structure, which was formed by the unique intermolecular pi overlap directed toward three directions from the triangular-shape NDI-Delta radical anions: Electron paramagnetic resonance and static magnetic measurements confirmed the radical anion state of NDI-Delta and indicated an antiferromagnetic intermolecular interaction With the Weiss constant of theta = -10 K. The band structure calculation suggested characteristic features of the present material, such as a metallic ground state, Dirac cones, and flat bands.

DOI： 10.1021/jacs.5b04180

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Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：ROYAL SOC CHEMISTRY  

A heterocyclic thiazyl diradical, bis(1,2,3,5-dithiadiazolyl)-4,4'-biphenylene (1), was synthesized, and its structural and thermodynamic properties were characterized. This compound exhibits unique spatially inhomogeneous, first-order phase transitions at 306 and 359 K, in a stepwise fashion. The unit cell in the high-temperature phase above 359 K consists of four regular pi-stacking columns with the same stacking manners having a uniform interplanar distance d. These four columns are connected by intermolecular S center dot center dot center dot S and S center dot center dot center dot N contacts between the thiazyl radical moieties, but the molecular planes are shifted by a distance of d/4 due to a steric hindrance between the bulky biphenylene moieties. Below 359 K, three of the four stacking columns exhibit structural transitions toward zigzag chain structures, formed by an alternating dimerization between the radical moieties, while one column maintains the uniform pi stacking. In the low-temperature phase below 306 K, the last column finally exhibits the radical dimerization toward a zigzag chain structure. These unique phase transitions in 1 can be understood in terms of the stepwise transitions from a "dimer liquid" to a "dimer solid" through a "dimer soliton phase".

DOI： 10.1039/c5tc01410g

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：NATURE PUBLISHING GROUP  

The neutral radical 1,3,5-trithia-2,4,6-triazapentalenyl (TTTA) is a prototype of molecule-based bistable materials. TTTA crystals undergo a first-order phase transition between their low-temperature diamagnetic and high-temperature paramagnetic phases, with a large hysteresis loop that encompasses room temperature. Here, based on ab initio molecular dynamics simulations and new X-ray measurements, we uncover that the regular stacking motif of the high-temperature polymorph is the result of a fast intra-stack pair-exchange dynamics, whereby TTTA radicals continually exchange the adjacent TTTA neighbour (upper or lower) with which they form an eclipsed dimer. Such unique dynamics, observed in the paramagnetic phase within the whole hysteresis loop, is the origin of a significant vibrational entropic gain in the low-temperature to high-temperature transition and thereby it plays a key role in driving the phase transition. This finding provides a new key concept that needs to be explored for the rational design of novel molecule-based bistable magnetic materials.

DOI： 10.1038/ncomms5411

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Language：Japanese   Publishing type：Research paper (scientific journal)   Publisher：AMER CHEMICAL SOC  

Thin films of a thiazyl biradical, naphtho[2,1-d:6,5-d']bis([1,2,3]dithiazole), abbreviated as NT, exhibit nonlinear optical properties with a large third-order nonlinear susceptibility of 2.1 X 10(-11) esu. The electroabsorption and low-temperature-absorption measurements reveal a series of degenerate electronic states, which is probably caused by the biradical character of NT. It is concluded that this degeneracy should enhance the third-order nonlinear optical properties.

DOI： 10.1021/jp4093332

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：CHEMICAL SOC JAPAN  

Heterocyclic thiazyl radicals possess unique chemical and physical properties as building blocks for molecule-based conductors and magnetic materials. They do not need protecting groups on their molecular skeletons, and the lack of such substituents permits close packing in the solid state. Moreover, thiazyl radical solids often involve a multidimensional network consisting of pi-pi overlaps and S center dot center dot center dot N contacts. The electronic structures of the thiazyl radicals can be compared to highly-correlated electron systems. In this account, we describe various electron-transfer processes in the solids of the thiazyl radicals, which manifest themselves by external stimuli such as temperature change, electric field, and photoillumination.

DOI： 10.1246/bcsj.20130248

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：AMER CHEMICAL SOC  

The crystal structures and magnetic properties of seven kinds of [1,2,51thiadiazolO[3,4-f] [1,10]phenanthroline 1,1-dioxide (tdapO(2)) radical anion salts, namely, K-tdap02, Ktdap02.0.5MeCN, K.(tdapO(2))(2), Rb.(tdap02)2, Cs"(tdap02)6.C104, (NH4)2-tdap021, and Hppda.tdap02.MeCN, were investigated. Single-crystal X-ray analyses of these radical anion salts revealed formation of ir-stacking columns and. the presence of intercolumnar coordination bonding or hydrogen 0.1 ".bonding. The intermolecular magnetic coupling constants in these salts range from strong antiferromagnetic (J/kB = 310 K) to ferromagnetic (J/kB = 24 K). Ab initio calculations performed on the nearest-neighbor radical pairs in the z-stacking columns suggested that the magnetic interactions are strongly governed by the,overlap between the two anionic radical species and well explain the observed ferromagnetic and antiferromagnetic interactions. In addition, calculations of a hypothetical, oxygen less tdap analogue suggested that the presence of oxygen in tclapO(2) significantly reduces the hopping integral and enhances the probability of ferromagnetic.. 'interaction.

DOI： 10.1021/ic401078z

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Language：Japanese   Publisher：The Vacuum Society of Japan  

  Most research in the field of organic electronics has focused on π-conjugated molecules with a closed-shell configuration, which accommodate their π-electrons in only bonding orbitals and are consequently quite stable. In general, closed-shell molecules have wide energy gaps, and they have significantly weaker intermolecular interactions. In contrast, recently organic biradicals have attracted considerable attention, owing to their interesting physical properties, <i>e.g.</i>, a small energy gap and strong intermolecular interactions. Organic biradical molecules are composed of a pair of organic radicals that possess an open-shell configuration. Owing to their radical nature, biradical molecules exhibit unusual physical properties such as those listed above. This article is a review of our recent study on the electronic structure of two different types of organic biradical molecules that have potential as new materials for manufacturing electronic devices. In particular, our results show that organic biradicals are expected to form a new class of materials for use in organic electronics as new building blocks for highly ordered organic semiconducting films with wide energy band dispersion widths and a narrow energy gap.<br>

DOI： 10.3131/jvsj2.56.32

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Language：Japanese   Publishing type：Research paper (scientific journal)   Publisher：AMER CHEMICAL SOC  

A novel phenanthlorine derivative, [1,2,5]thiadiazolo[3,4-f][1,10]phenanthroline 1,1-dioxide (tdapO(2)), was prepared to act as a radical-anion building block for coordination polymers. The crystal structures and magnetic properties of the monovalent and mixed-valent radical-anion salts K center dot tdapO(2) and K center dot(tdapO(2))(2) were elucidated and confirm the possibility of tdapO(2) to act as a bridging ligand and its capability to exhibit magnetic ordering at 15 K.

DOI： 10.1021/ic201966t

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：AMER PHYSICAL SOC  

As a significant drawback to organic electronics, poor mobility in organic materials makes it difficult for carriers to make long trips across thin film devices. In the present work, we show that a short carrier trip or even charge displacement can contribute to the functioning of optoelectronics without being influenced by the poor carrier mobility. Our findings are based on analysis of the current-voltage and capacitance-voltage characteristics, as well as the anomalous transient photocurrent of the photocells of a radical material, 4&apos;4-bis(1,2,3,5-dithiadiazolyl). This photoinduced transient current was successfully analyzed based on the total current equation and was interpreted in terms of the polarization current induced by charge displacement in the films. This mechanism provides preliminary information with respect to the development of methods for high-speed organic optoelectronic conversion.

DOI： 10.1103/PhysRevB.84.205329

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：ELSEVIER SCIENCE BV  

Thin films of interacting dimers of 4,4&apos;-bis(1,2,3,5-dithiadiazolyl), sandwiched by ITO and Al, exhibit an anomalous transient current, due to a significant imbalance between the hole and electron mobilities and bulk polarization. We propose a new operational principle for organic optoelectronic conversion systems, which efficiently generates alternating photocurrent without being affected by the disadvantages of organic materials, such as poor mobility. (C) 2009 Elsevier B.V. All rights reserved.

DOI： 10.1016/j.cplett.2009.11.013

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：WILEY-V C H VERLAG GMBH  

DOI： 10.1002/anie.200900472

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Language：Japanese   Publishing type：Research paper (scientific journal)   Publisher：ROYAL SOC CHEMISTRY  

We prepared an iron(II) spin crossover complex with a new ligand, [1,2,5] thiadiazolo[3,4-f][1,10] phenanthroline, which is a 1,10-phenanthroline analogue annulated with a thiadiazole moiety. X-Ray crystal analysis indicated a 3D network structure formed by short S center dot center dot center dot S contacts, and magnetic measurements revealed a broad transition above room temperature.

DOI： 10.1039/b906845g

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：ROYAL SOC CHEMISTRY  

The electronic structure of the thiazyl diradical, 4,4'-bis(1,2,3,5-dithiadiazolyl) (BDTDA), has been investigated by ultraviolet photoemission spectroscopy. Stacked BDTDA dimers showed an energy band dispersion of about 0.3 eV for the highest occupied molecular orbital in the direction of the surface normal of the BDTDA solid film. The pi-orbital overlap between the stacked dimers therefore evolves into a quasi one-dimensional energy band along the dimer stacking direction.

DOI： 10.1039/b916396d

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：WILEY-V C H VERLAG GMBH  

DOI： 10.1002/chem.200800519

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：ELSEVIER SCIENCE SA  

Selective preparation and characterization of a series of heteroleptic thiolate complexes of iron(II) are described. The compounds were synthesized by treatment of iron bis-amide Fe{N(SiMe3)(2)}(2) (1) with 1 equiv. of terphenyl thiols HS(2,6-(aryl)(2)C6H3) followed by addition of another equivalent of different thiol. An amide-thiolate intermediate [{(Me3Si)(2)N}Fe](2)(mu-SDpp)(2) (2; Dpp = 2,6-Ph2C6H3) was isolated from the 1:1 reaction of I and HSDpp. The X-ray crystal structures of all new thiolate complexes have been determined. The compounds crystallize as monomers or dimers, dependent on the substituents. They consist of distorted tetrahedral or trigonal-pla nar iron centers with weak interactions between the aromatic rings of thiolate ligands, where the Fe-C(arene) contact is 2.272(2) A at shortest. The stronger iron-arene interaction appears to induce more pyramidalized geometry at the iron center. (C) 2007 Elsevier B.V. All rights reserved.

DOI： 10.1016/j.jorganchem.2007.06.027

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：CHEMICAL SOC JAPAN  

Twelve-membered cyclic diethynylphosphine derivatives (R(2)(1)SiCdropC-R(2)PCdropC)(2) (1a: R-1 = R-2 = Ph; 1b: R-1 = Ph, R-2 = t-Bu; 1c: R-1 = i-Pr, R-2 = Ph) have been synthesized as a novel cyclic phosphine ligand including potentially reactive acetylene and silane moieties. Compounds 1a and 1b were formed as a mixture of cis- and trans-isomers, while an only trans-isomer was obtained for 1c. X-ray structural analysis revealed planar skeletal structures of the trans-isomers of 1a-c.

DOI： 10.1246/cl.2003.1024

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：ROYAL SOC CHEMISTRY  

Novel hetero-halogenated TTFs containing both chlorine and iodine atoms were prepared and their unique characters based on the halogen atoms were examined.

DOI： 10.1039/b310822h

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：ELSEVIER SCIENCE SA  

Treatment of Mn(CO)(5)SiTol(2)(p)H (2) with an excess of LiAlH4, NaBH4, or NaBH3(CN) in THF at room temperature gave hydrosilane H-SiTol(2)(p)H in high yield together with Mn-2(CO)(10). No reduction of CO ligands was observed. On the other hand, treatment of 2 with an excess of Red-Al (= Na[(CH3OCH3CH2O)(2)AlH2]) in toluene and subsequent addition of aqueous acidic solution afforded alkylsilanols (CH3)SiTol(2)(p)(OH) and (C2H5)SiTol(2)(p)(OH). Treatment of the reaction mixture of 2 and Red-Al with LiAlH4 in diethyl ether instead of hydrolysis gave alkylhydrosilanes (CH3)SiTol(2)(p)H and (C2H5)SiTol(2)(p)H. The methyl and ethyl groups on silicon originate from the CO ligands in 2. These products clearly demonstrate that not only the Si-C coupling, but also C-C coupling occurs efficiently in this reaction. (C) 2002 Elsevier Science B.V. All rights reserved.

DOI： 10.1016/S0022-328X(02)01188-9

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：ELSEVIER SCIENCE SA  

The anionic ruthenium and iron complexes Li[(eta(5)-C5Me5)M(CO)(2)] (M = Ru (1-Ru), Fe (1-Fe)) were generated by deprotonation of the transition metal hydride (eta(5)-C5Me5)M(CO)(2)H with n-BuLi in tetrahydrofuran (THF). The reaction proceeded at -45 degreesC immediately. Reactions of 1 with various electrophiles (Me3SiCl, (p)Tol(2)HSiCl, Me2SiCl2, MeSiCl3, SiCl4, Me3SiSiMe2Cl, and Ph2GeCl2) afforded the corresponding nucleophilic substitution products (eta(5)-C5Me5)M(CO)(2)ER3 (E = Si, Ge) via salt-elimination. (C) 2002 Elsevier Science B.V. All rights reserved.

DOI： 10.1016/S0022-328X(01)01373-0

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：AMER CHEMICAL SOC  

Treatment of CpFe(CO)(2)SiR3 (Cp = eta(5)-C5H5; R-3 = (p)Tol(2)Cl, (p)Tol(2)H, (p)Tol(2)Me, MePh (1-Nap), and (n-C5H11)(2)H; 1-Nap = 1-naphthyl) with LiAlH4 in ether or THF at room temperature gave CH3SiR3 as the major product in moderate to high yield together with HSiR3. Reaction of CpFe(CO)(2)SiMes(2)H with LiAlH4 afforded only H(2)SiMes(2). Labeling experiments using LiAlD4 gave the deuterated methylsilanes. These results proved that the hydrogen source for the methyl group is LiAlH4. Furthermore, the reduction of CpFe(*CO)(2)Si(p)Tol(2)R' (*C = C-13 enriched; R' = H,Me) produced *CH(3)Si(p)Tol(2)R' where the methyl group introduced on Si was C-13-enriched. These experimental results suggested that the carbonyl ligand was reduced by LiAlH4 and coupled with the silyl group to give the methylsilane. Cp*Fe(CO)(2)Si(p)Tol(2)H (Cp* = eta(5)-C5Me5), having a Cp* ligand which is bulkier and more electron-donating than a Cp ligand, did not react with LiAlH4 at room temperature, but it did so at 50 degrees C to give CH(3)Si(p)Tol(2)H and HSi(p)Tol(2)H, probably because nucleophilic attack of LiAlH4 at a carbonyl ligand was retarded both sterically and electronically by the Cp* ligand. When the :reactions were performed in sealed NMR tubes and monitored by NMR spectroscopy, the signals due to the anionic complexes Li+[CpFe(CO)(CH3)Si(p)Tol(2)R'](-) were observed in addition to those of silane products. These anionic complexes are considered not to be intermediates but to be byproducts because the anionic complexes did not change to methylsilanes on heating. The anionic complexes reacted with MeOH and Mel to give hydrosilanes HSi(p)Tol(2)R' and methylsilanes CH(3)Si(p)Tol(2)R', respectively.

DOI： 10.1021/om9802111

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：CHEMICAL SOC JAPAN  

Treatment of CpFe(CO)(2)SiR3 (R-3 = (pTol)(2)H, ((p)Tol)(2)Me, MePh(1-Nap); 1-Nap = 1-naphthyl) with LiAlH4 in ether or THF at room temperature gave CH3SiR3 as a major product in moderate to high yield. The labeling experiments using LiAlD4 and CpFe((CO)-C-13)(2)SiR(pTol)(2) (R = H, Me) proved unambiguously that the carbonyl ligand is reduced with LiAlH4 and coupled with the silyl group to give the methylsilane.

DOI： 10.1246/cl.1997.805

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Language：Japanese   Publishing type：Article, review, commentary, editorial, etc. (scientific journal)  

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Language：Japanese   Publisher：一般社団法人 日本物理学会  

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Language：Japanese   Publisher：The Physical Society of Japan (JPS)  

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Language：Japanese   Publisher：The Physical Society of Japan (JPS)  

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