担当区分：最終著者,　責任著者   記述言語：英語   掲載種別：研究論文（学術雑誌）   出版者・発行元：Environmental Research Letters  

East and South Asia are major hotspots of crop straw burning worldwide, with profound impacts on air quality and climate change. The Northeast China Plain (NECP) and Punjab, India, are two of the most fertile areas for crop production, which have large-scale agricultural fires during post-harvest seasons. Leveraging established fire-emission databases and satellite-retrieved agricultural fire spots, we show that, while the years 2018 and 2019 recorded low agricultural fire emissions in both the NECP and Punjab, probably due to the implementation of crop straw sustainable management, fire emissions markedly rebounded in 2020, reaching about 190% and 150% of 2019 levels, respectively. The COVID-19 lockdown measures somewhat disrupted eco-friendly crop straw management through restrictions on labor and transportation availability, such that farmers may have had to burn off crop wastes to clear up the land. We further demonstrate that the increased fire emissions in the NECP resulted in serious particulate matter pollution during the fire season in spring 2020, as opposed to considerable decreases in particles from fossil fuel emissions caused by the COVID-19 lockdown. This study suggests the unintended impacts of the COVID-19 pandemic on the agricultural sector and human health.

DOI： 10.1088/1748-9326/ac9e69

DOI： 10.1088/1748-9326/ac9e69

Web of Science

Scopus

記述言語：英語   掲載種別：研究論文（学術雑誌）   出版者・発行元：Nature Communications  

Biomass burning (BB) is a major source of aerosols that remain the most uncertain components of the global radiative forcing. Current global models have great difficulty matching observed aerosol optical depth (AOD) over BB regions. A common solution to address modelled AOD biases is scaling BB emissions. Using the relationship from an ensemble of aerosol models and satellite observations, we show that the bias in aerosol modelling results primarily from incorrect lifetimes and underestimated mass extinction coefficients. In turn, these biases seem to be related to incorrect precipitation and underestimated particle sizes. We further show that boosting BB emissions to correct AOD biases over the source region causes an overestimation of AOD in the outflow from Africa by 48%, leading to a double warming effect compared with when biases are simultaneously addressed for both aforementioned factors. Such deviations are particularly concerning in a warming future with increasing emissions from fires.

DOI： 10.1038/s41467-022-33680-4

DOI： 10.1038/s41467-022-33680-4

Web of Science

Scopus

PubMed

担当区分：最終著者,　責任著者   記述言語：英語   掲載種別：研究論文（学術雑誌）   出版者・発行元：Geophysical Research Letters  

Formation of secondary organic aerosols (SOA) through the atmospheric oxidation of organic vapors has potential to enable particle growth to cloud condensation nuclei (CCN)-relevant sizes. In this work, we constrain a global aerosol model by using aircraft measurements to reveal the global importance of SOA formation in CCN production. Our improved model, with explicit size-resolved aerosol microphysics and parametrizations of semivolatile organic oxidation products, presents a state-of-the-art performance in simulating both particle number concentrations and organic aerosol concentrations dominated (80–95%) by SOA in the remote atmosphere, which have been challenges in previous modeling studies. The SOA formation in concert with aerosol nucleation contributes to more than 50% of CCN concentrations in those pristine environments featuring low background aerosol concentrations. We estimate that the SOA-derived CCN alters the magnitude of cloud radiative forcing by ∼0.1 W m−2. Our findings underscore the necessity for aerosol-climate models to represent controls on CCN concentrations by SOA production.

DOI： 10.1029/2022GL100543

DOI： 10.1029/2022GL100543

Web of Science

Scopus

記述言語：英語   掲載種別：研究論文（学術雑誌）   出版者・発行元：Journal of Geophysical Research: Atmospheres  

Aerosols significantly affect Earth's radiation budget, thus influencing global climate. In the Arctic, sulfate aerosols are thought to have reduced the warming during the twentieth century. However, trends in past sulfate aerosols are poorly known, especially the aerosol sizes and compositions. Here, we analyze a high-resolution ice core from southeastern Greenland, comparing the seasonal deposition flux of large sulfate salt particles and small sulfur compounds, including non-neutralized sulfuric acid, between the anthropogenic sulfate maximum (1973–1975) and after sulfur emissions control (2010–2012). Between these periods, we find that the large-diameter (>0.4 μm) flux remains roughly unchanged, yet the small-diameter (<0.4 μm) aerosol flux significantly decreases. The results indicate that small sulfates were efficiently activated as cloud condensation nuclei during the 1970s, and thus likely increased cloud albedo, offsetting the warming.

DOI： 10.1029/2022JD036880

DOI： 10.1029/2022JD036880

Web of Science

Scopus

担当区分：筆頭著者,　責任著者   記述言語：英語   掲載種別：研究論文（学術雑誌）   出版者・発行元：Journal of Geophysical Research: Atmospheres  

Aerosols can modulate the Arctic climate through their interactions with radiation, clouds, and snow and ice surfaces. Atmospheric simulations of Arctic aerosols remain highly uncertain, for which the importance of aerosol microphysical properties and processes has not been properly evaluated. To identify the cause of this large uncertainty, we evaluate the variability ranges of aerosols in the Arctic resulting from uncertainties in various aerosol microphysical properties/processes, including particle size distributions at emission, particle mixing states, activation efficiency, and wet removal processes, by using a global climate-aerosol model Community Atmosphere Model with the Aerosol Two-dimensional bin module for foRmation and Aging Simulation. We find that the combined uncertainties associated with these multiple microphysical properties/processes yield a factor of 10–50 differences (maximum-to-minimum ratio) in the concentrations and radiative effects of aerosols in the Arctic. Black carbon shows the highest variability among aerosol species because its lower hygroscopicity and higher critical supersaturation cause the fraction of activation and wet removal during transport to be highly sensitive to the model treatment of aerosol and cloud microphysics. Aerosol-radiation-cloud interactions at the top of atmosphere vary from −0.40 to +0.30 W m−2 in the Arctic (from the preindustrial to present day) and can be positive or negative depending on the treatment of microphysical properties/processes. These results indicate that microphysical properties/processes are more important than previously thought in aerosol simulations in the Arctic and demonstrate that a better understanding and more sophisticated model representation of aerosol microphysical properties/processes are required to improve the accuracy of Arctic aerosol simulations and their impacts on climate.

DOI： 10.1029/2022JD036943

DOI： 10.1029/2022JD036943

Web of Science

Scopus

記述言語：英語   掲載種別：研究論文（学術雑誌）   出版者・発行元：Atmospheric Chemistry and Physics  

Global models are widely used to simulate biomass burning aerosol (BBA). Exhaustive evaluations on model representation of aerosol distributions and properties are fundamental to assess health and climate impacts of BBA. Here we conducted a comprehensive comparison of Aerosol Comparisons between Observations and Models (AeroCom) project model simulations with satellite observations. A total of 59 runs by 18 models from three AeroCom Phase-III experiments (i.e., biomass burning emissions, CTRL16, and CTRL19) and 14 satellite products of aerosols were used in the study. Aerosol optical depth (AOD) at 550 nm was investigated during the fire season over three key fire regions reflecting different fire dynamics (i.e., deforestation-dominated Amazon, Southern Hemisphere Africa where savannas are the key source of emissions, and boreal forest burning in boreal North America). The 14 satellite products were first evaluated against AErosol RObotic NETwork (AERONET) observations, with large uncertainties found. But these uncertainties had small impacts on the model evaluation that was dominated by modeling bias. Through a comparison with Polarization and Directionality of the Earth's Reflectances measurements with the Generalized Retrieval of Aerosol and Surface Properties algorithm (POLDER-GRASP), we found that the modeled AOD values were biased by -93 % to 152 %, with most models showing significant underestimations even for the state-of-the-art aerosol modeling techniques (i.e., CTRL19). By scaling up BBA emissions, the negative biases in modeled AOD were significantly mitigated, although it yielded only negligible improvements in the correlation between models and observations, and the spatial and temporal variations in AOD biases did not change much. For models in CTRL16 and CTRL19, the large diversity in modeled AOD was in almost equal measures caused by diversity in emissions, lifetime, and the mass extinction coefficient (MEC). We found that in the AeroCom ensemble, BBA lifetime correlated significantly with particle deposition (as expected) and in turn correlated strongly with precipitation. Additional analysis based on Cloud-Aerosol LIdar with Orthogonal Polarization (CALIOP) aerosol profiles suggested that the altitude of the aerosol layer in the current models was generally too low, which also contributed to the bias in modeled lifetime. Modeled MECs exhibited significant correlations with the Ångström exponent (AE, an indicator of particle size). Comparisons with the POLDER-GRASP-observed AE suggested that the models tended to overestimate the AE (underestimated particle size), indicating a possible underestimation of MECs in models. The hygroscopic growth in most models generally agreed with observations and might not explain the overall underestimation of modeled AOD. Our results imply that current global models contain biases in important aerosol processes for BBA (e.g., emissions, removal, and optical properties) that remain to be addressed in future research. Copyright:

DOI： 10.5194/acp-22-11009-2022

DOI： 10.5194/acp-22-11009-2022

Web of Science

Scopus

記述言語：英語   掲載種別：研究論文（学術雑誌）   出版者・発行元：Geophysical Research Letters  

Anthropogenic emission is an important component of the present-day iron cycle yet its long-term impacts on climate are poorly understood. Iron mineralogy strongly affects its radiative and oceanic interactions and was unrepresented in previous studies. We perform simulations using a mineralogy-based inventory and an atmospheric transport model and estimate the 1850–2010 global mean direct radiative forcing (DRF) to be +0.02 to +0.10 W/m2. We estimate that the CO2 sequestration of 0.2–13 ppmv over the last 150 years due to enhanced phytoplankton productivity by anthropogenic iron deposition causes an avoided CO2 forcing of −0.002 to −0.16 W/m2. While globally small, these impacts can be higher in specific regions; the anthropogenic DRF is +0.5 W/m2 over areas with more coal combustion and metal smelting, and anthropogenic soluble iron sustains >10% of marine net primary productivity in the high-latitude North Pacific Ocean, a region vulnerable to stratification due to climate change.

DOI： 10.1029/2022GL099323

DOI： 10.1029/2022GL099323

Web of Science

Scopus

担当区分：筆頭著者,　責任著者   記述言語：英語   掲載種別：研究論文（学術雑誌）   出版者・発行元：Atmospheric Chemistry and Physics  

Black carbon (BC) particles in the Arctic contribute to rapid warming of the Arctic by heating the atmosphere and snow and ice surfaces. Understanding the source contributions to Arctic BC is therefore important, but they are not well understood, especially those for atmospheric and snow radiative effects. Here we estimate simultaneously the source contributions of Arctic BC to near-surface and vertically integrated atmospheric BC mass concentrations (MBC-SRF and MBC-COL), BC deposition flux (MBC-DEP), and BC radiative effects at the top of the atmosphere and snow surface (REBC-TOA and REBC-SNOW) and show that the source contributions to these five variables are highly different. In our estimates, Siberia makes the largest contribution to MBC-SRF, MBC-DEP, and REBC-SNOW in the Arctic (defined as >70° N), accounting for 70 %, 53 %, and 41 %, respectively. In contrast, Asia's contributions to MBC-COL and REBC-TOA are largest, accounting for 37 % and 43 %, respectively. In addition, the contributions of biomass burning sources are larger (29 %-35 %) to MBC-DEP, REBC-TOA, and REBC-SNOW, which are highest from late spring to summer, and smaller (5.9 %-17 %) to MBC-SRF and MBC-COL, whose concentrations are highest from winter to spring. These differences in source contributions to these five variables are due to seasonal variations in BC emission, transport, and removal processes and solar radiation, as well as to differences in radiative effect efficiency (radiative effect per unit BC mass) among sources. Radiative effect efficiency varies by a factor of up to 4 among sources (1471-5326 W g-1) depending on lifetimes, mixing states, and heights of BC and seasonal variations of emissions and solar radiation. As a result, source contributions to radiative effects and mass concentrations (i.e., REBC-TOA and MBC-COL, respectively) are substantially different. The results of this study demonstrate the importance of considering differences in the source contributions of Arctic BC among mass concentrations, deposition, and atmospheric and snow radiative effects for accurate understanding of Arctic BC and its climate impacts.

DOI： 10.5194/acp-22-8989-2022

DOI： 10.5194/acp-22-8989-2022

Web of Science

Scopus

担当区分：責任著者   記述言語：英語   掲載種別：研究論文（学術雑誌）   出版者・発行元：npj Climate and Atmospheric Science  

The atmospheric deposition of soluble (bioaccessible) iron enhances ocean primary productivity and subsequent atmospheric CO2 sequestration in iron-limited ocean basins, especially the Southern Ocean. While anthropogenic sources have been recently suggested to be important in some northern hemisphere oceans, the role in the Southern Ocean remains ambiguous. By comparing multiple model simulations with the new aircraft observations for anthropogenic iron, we show that anthropogenic soluble iron deposition flux to the Southern Ocean could be underestimated by more than a factor of ten in previous modeling estimates. Our improved estimate for the anthropogenic iron budget enhances its contribution on the soluble iron deposition in the Southern Ocean from about 10% to 60%, implying a dominant role of anthropogenic sources. We predict that anthropogenic soluble iron deposition in the Southern Ocean is reduced substantially (30‒90%) by the year 2100, and plays a major role in the future evolution of atmospheric soluble iron inputs to the Southern Ocean.

DOI： 10.1038/s41612-022-00250-w

DOI： 10.1038/s41612-022-00250-w

Web of Science

Scopus

記述言語：英語   掲載種別：研究論文（学術雑誌）   出版者・発行元：Earth and Planetary Science Letters  

Chemical proxy data from ice cores provide information for understanding environmental changes. Despite large climate shifts, the flux of sulfate onto the ice in Antarctica has remained relatively stable over glacial-interglacial cycles. However, the mechanism behind the stable flux is controversial because of a lack of evidence for changes in multiple source emissions. Here, we present the sulfur isotopic record in the Antarctic Dome Fuji ice core, which provides a new constraint on the interpretation of sulfate aerosols. During the Last Glacial Maximum (LGM), the sulfur isotope ratio was depleted compared to that during the Holocene and was negatively correlated with terrestrial contributions. The isotope data suggest that the contributions from terrestrial gypsum were enhanced during the LGM. A potential source area for gypsum in the Antarctic ice core is the high-altitude region around the Atacama Desert, although other regions cannot be excluded. These results suggest that the salts in deserts should be considered a terrestrial source of Antarctic sulfate during the LGM.

DOI： 10.1016/j.epsl.2021.117299

Scopus

記述言語：英語   掲載種別：研究論文（学術雑誌）   出版者・発行元：Atmospheric Chemistry and Physics  

Vertical profiles of the mass concentration of black carbon (BC) were measured at altitudes up to 5 km during the PAMARCMiP (Polar Airborne Measurements and Arctic Regional Climate Model simulation Project) aircraft-based field experiment conducted around the northern Greenland Sea (Fram Strait) during March and April 2018 from operation base Station Nord (81.6'N, 16.7'W). Median BC mass concentrations in individual altitude ranges were 7-18 ng m-3 at standard temperature and pressure at altitudes below 4.5 km. These concentrations were systematically lower than previous observations in the Arctic in spring, conducted by ARCTAS-A in 2008 and NETCARE in 2015, and similar to those observed during HIPPO3 in 2010. Column amounts of BC for altitudes below 5 km in the Arctic (>66.5'N; COLBC), observed during the ARCTAS-A and NETCARE experiments, were higher by factors of 4.2 and 2.7, respectively, than those of the PAMARCMiP experiment. These differences could not be explained solely by the different locations of the experiments. The year-to-year variation of COLBC values generally corresponded to that of biomass burning activities in northern midlatitudes over western and eastern Eurasia. Furthermore, numerical model simulations estimated the year-to-year variation of contributions from anthropogenic sources to be smaller than 30 %-40 %. These results suggest that the year-to-year variation of biomass burning activities likely affected BC amounts in the Arctic troposphere in spring, at least in the years examined in this study. The year-to-year variations in BC mass concentrations were also observed at the surface at high Arctic sites Ny-Ålesund and Utqiävik (formerly known as Barrow, the location of Barrow Atmospheric Baseline Observatory), although their magnitudes were slightly lower than those in COLBC. Numerical model simulations in general successfully reproduced the observed COLBC values for PAMARCMiP and HIPPO3 (within a factor of 2), whereas they markedly underestimated the values for ARCTAS-A and NETCARE by factors of 3.7-5.8 and 3.3-5.0, respectively. Because anthropogenic contributions account for nearly all of the COLBC (82 %-98 %) in PAMARCMiP and HIPPO3, the good agreement between the observations and calculations for these two experiments suggests that anthropogenic contributions were generally well reproduced. However, the significant underestimations of COLBC for ARCTAS-A and NETCARE suggest that biomass burning contributions were underestimated. In this study, we also investigated plumes with enhanced BC mass concentrations, which were affected by biomass burning emissions, observed at 5 km altitude. Interestingly, the mass-averaged diameter of BC (core) and the shell-to-core diameter ratio of BC-containing particles in the plumes were generally not very different from those in other air samples, which were considered to be mostly aged anthropogenic BC. These observations provide a useful basis to evaluate numerical model simulations of the BC radiative effect in the Arctic region in spring.

DOI： 10.5194/acp-21-15861-2021

Web of Science

Scopus

担当区分：責任著者   記述言語：英語   掲載種別：研究論文（学術雑誌）  

記述言語：英語   掲載種別：研究論文（学術雑誌）   出版者・発行元：Atmospheric Chemistry and Physics  

Aerosol-induced absorption of shortwave radiation can modify the climate through local atmospheric heating, which affects lapse rates, precipitation, and cloud formation. Presently, the total amount of aerosol absorption is poorly constrained, and the main absorbing aerosol species (black carbon (BC), organic aerosols (OA), and mineral dust) are diversely quantified in global climate models. As part of the third phase of the Aerosol Comparisons between Observations and Models (AeroCom) intercomparison initiative (AeroCom phase III), we here document the distribution and magnitude of aerosol absorption in current global aerosol models and quantify the sources of intermodel spread, highlighting the difficulties of attributing absorption to different species. In total, 15 models have provided total present-day absorption at 550nm (using year 2010 emissions), 11 of which have provided absorption per absorbing species. The multi-model global annual mean total absorption aerosol optical depth (AAOD) is 0.0054 (0.0020 to 0.0098; 550nm), with the range given as the minimum and maximum model values. This is 28% higher compared to the 0.0042 (0.0021 to 0.0076) multi-model mean in AeroCom phase II (using year 2000 emissions), but the difference is within 1 standard deviation, which, in this study, is 0.0023 (0.0019 in Phase II). Of the summed component AAOD, 60% (range 36%-84%) is estimated to be due to BC, 31% (12%-49%) is due to dust, and 11% (0%-24%) is due to OA; however, the components are not independent in terms of their absorbing efficiency. In models with internal mixtures of absorbing aerosols, a major challenge is the lack of a common and simple method to attribute absorption to the different absorbing species. Therefore, when possible, the models with internally mixed aerosols in the present study have performed simulations using the same method for estimating absorption due to BC, OA, and dust, namely by removing it and comparing runs with and without the absorbing species. We discuss the challenges of attributing absorption to different species; we compare burden, refractive indices, and density; and we contrast models with internal mixing to models with external mixing. The model mean BC mass absorption coefficient (MAC) value is 10.1 (3.1 to 17.7)m2g-1 (550nm), and the model mean BC AAOD is 0.0030 (0.0007 to 0.0077). The difference in lifetime (and burden) in the models explains as much of the BC AAOD spread as the difference in BC MAC values. The difference in the spectral dependency between the models is striking. Several models have an absorption Ångstrøm exponent (AAE) close to 1, which likely is too low given current knowledge of spectral aerosol optical properties. Most models do not account for brown carbon and underestimate the spectral dependency for OA.

DOI： 10.5194/acp-21-15929-2021

Web of Science

Scopus

担当区分：筆頭著者,　責任著者   記述言語：英語   掲載種別：研究論文（学術雑誌）   出版者・発行元：Journal of Climate  

Black carbon (BC) aerosol particles in the Arctic heat the atmosphere and snow/ice surfaces and may strengthen the snow-albedo feedback that amplifies Arctic warming. Model simulations of BC concentrations in the Arctic depend strongly on the representation of microphysical processes such as aging, activation, and wet removal. Most BC modeling studies have classified BC particles into hydrophobic BC, which cannot form cloud droplets, and hydrophilic BC, which can form cloud droplets, by assuming a globally constant critical supersaturation threshold value (Sthre), without considering its consistency with cloud maximum supersaturation (Smax). Here we show that it is essential to consider the consistency of Sthre with Smax in global model simulations to reduce uncertainties in near-surface ambient BC concentrations in the Arctic. Previous studies often obtained good agreement between simulated and observed near-surface Arctic BC mass concentrations when a low Sthre (;0.1%) was assumed in their models. However, this Sthre may be too low (activation and wet removal of BC may be underestimated) for the Arctic, because some recent observations and our model simulations suggest that Smax may actually be higher (;0.3%) there. We also demonstrate that spatially varying Sthre values and their consistency with Smax, which previous studies did not consider, must be represented in models for more accurate estimation of BC budget in the Arctic. Because both Smax and BC-aging speed depend on climatic conditions, our findings are an important step toward better simulations of BC impacts on past, present, and future Arctic climates.

DOI： 10.1175/JCLI-D-20-0994.1

Scopus

記述言語：英語   掲載種別：研究論文（学術雑誌）   出版者・発行元：Journal of Advances in Modeling Earth Systems  

Biases in aerosol optical depths (AOD) and land surface albedos in the AeroCom models are manifested in the top-of-atmosphere (TOA) clear-sky reflected shortwave (SW) fluxes. Biases in the SW fluxes from AeroCom models are quantitatively related to biases in AOD and land surface albedo by using their radiative kernels. Over ocean, AOD contributes about 25% to the (Formula presented.) S– (Formula presented.) N mean SW flux bias for the multi-model mean (MMM) result. Over land, AOD and land surface albedo contribute about 40% and 30%, respectively, to the (Formula presented.) S– (Formula presented.) N mean SW flux bias for the MMM result. Furthermore, the spatial patterns of the SW flux biases derived from the radiative kernels are very similar to those between models and CERES observation, with the correlation coefficient of 0.6 over ocean and 0.76 over land for MMM using data of 2010. Satellite data used in this evaluation are derived independently from each other, consistencies in their bias patterns when compared with model simulations suggest that these patterns are robust. This highlights the importance of evaluating related variables in a synergistic manner to provide an unambiguous assessment of the models, as results from single parameter assessments are often confounded by measurement uncertainty. Model biases in land surface albedos can and must be corrected to accurately calculate TOA flux. We also compare the AOD trend from three models with the observation-based counterpart. These models reproduce all notable trends in AOD except the decreasing trend over eastern China and the adjacent oceanic regions due to limitations in the emission data set.

DOI： 10.1029/2021MS002584

Web of Science

Scopus

担当区分：責任著者   記述言語：英語   掲載種別：研究論文（学術雑誌）   出版者・発行元：Journal of Geophysical Research: Atmospheres  

Mineral dust affects the microphysical and radiative properties of mixed-phase clouds and hence the radiative balance of the Earth by acting as ice nucleating particles (INPs). However, the importance of Asian dust as INPs is not well understood. In this study, we examined the contribution of Asian dust to global dust INPs and its effect on cloud radiative forcing (CRF) using a global aerosol-climate model with an ice nucleation parameterization that links INP number concentrations to ambient temperature and dust number concentrations. Our model well reproduces INP number concentrations measured over the Tokyo Metropolitan area in Japan during May 2017, when Asian dust was transported to Japan. Our simulation for the years 2013–2017 shows that Asian dust extends from its source regions (e.g., the Gobi and Taklimakan Deserts) to the North Pacific, North America, and the Arctic. Notably, Asian dust is transported to higher altitudes (i.e., to temperature regimes relevant for the formation of mixed-phase clouds) more efficiently than dust from other regions. The annual-mean simulated contribution of Asian dust to global dust INPs is 15%, which is 4.4 times higher than its contribution to global atmospheric dust loading (3.4%). These characteristics of Asian dust show its high potential to act as INPs in mixed-phase clouds. Sensitivity simulations show that Asian dust INPs have a positive net CRF of 0.054–0.19 W m−2 in East Asia and the North Pacific during 2013–2017 (cf. 0.092–1.0 W m−2 for dust from other regions).

DOI： 10.1029/2020JD034263

Web of Science

Scopus

記述言語：英語   掲載種別：研究論文（学術雑誌）   出版者・発行元：Journal of Geophysical Research: Atmospheres  

Black carbon (BC) aerosol deposited in and onto Arctic snow increases the snow's absorption of solar radiation and accelerates snowmelt. Concentrations of BC in the Arctic atmosphere and snow are controlled by wet deposition; however, details of this process are poorly understood owing to the scarcity of time-resolved measurements of BC in hydrometeors. We measured mass concentrations of BC in hydrometeors (CMBC) and in air (MBC) with 16% and 15% accuracies, respectively, at Ny-Ålesund, Svalbard during 2012–2019. Median monthly MBC and CMBC values showed similar seasonal variations, being high in winter-spring and low in summer. Median monthly BC wet deposition mass flux (FMBC) was highest in winter and lowest in summer, associated with seasonal patterns of CMBC and precipitation. Seasonally averaged BC size distributions in hydrometeors were similar except for summer. Measurements of MBC and CMBC in spring 2017 showed a size-independent removal efficiency, indicating that BC-containing particles were efficiently activated into cloud droplets. These observations at Ny-Ålesund were compared with observations at Barrow, Alaska, during 2013–2017. The near-surface MBC at Ny-Ålesund and Barrow had similar seasonal patterns; however, the two sites differed in CMBC and FMBC. In summer, CMBC was low at Ny-Ålesund but moderate at Barrow, likely reflecting differences in MBC in the lower troposphere. Seasonally averaged BC size distributions in hydrometeors were similar at both sites, suggesting that average BC size distributions are similar in the Arctic lower troposphere. The efficiency of BC removal tends to be size-independent during transport, leading to the observed similarity.

DOI： 10.1029/2020JD034110

Web of Science

Scopus

担当区分：最終著者,　責任著者   記述言語：英語   掲載種別：研究論文（学術雑誌）   出版者・発行元：Atmospheric Chemistry and Physics  

Anthropogenic emissions in China play an important role in altering the global radiation budget. Over the past decade, the strong clean-Air policies in China have resulted in substantial reductions of anthropogenic emissions of sulfur dioxide (SO2) and primary particulate matter, and air quality in China has consequently improved. However, the resultant aerosol radiative forcings have been poorly understood. In this study, we used an advanced global climate model integrated with the latest localized emission inventory to quantify the aerosol radiative forcings by the changes of anthropogenic emissions in China between 2008 and 2016. By comparing with multiple observation datasets, our simulations reproduced the considerable reductions of sulfate and black carbon (BC) mass loadings reasonably well over eastern China (the key region subject to stringent emission controls) during the period and accordingly showed a clear decline in both aerosol optical depth and absorption aerosol optical depth. The results revealed a regional annual mean positive direct radiative forcing (DRF) of C0.29Wm2 at the top of the atmosphere (TOA) due to the reduction of SO2 emissions. This positive aerosol radiative forcing was comprised of diminished sulfate scattering (C0.58Wm2), enhanced nitrate radiative effects (0.29Wm2), and could be completely offset by the concurrent reduction of BC emissions that induced a negative BC DRF of 0.33Wm2. Despite the small net aerosol DRF (0.05Wm2) at the TOA, aerosol radiation interactions could explain the surface brightening in China over the past decade. The overall reductions in aerosol burdens and associated optical effects mainly from BC and sulfate enhanced the regional annual mean downward solar radiation flux at the surface by C1.0Wm2 between 2008 and 2016. The enhancement was in general agreement with a long-Term observational record of surface energy fluxes in China. We also estimated that aerosol effects on cloud radiative forcings may have played a dominant role in the net aerosol radiative forcings at the TOA in China and over the northern Pacific Ocean during the study period. This study will facilitate more informed assessment of climate responses to projected emissions in the future as well as to sudden changes in human activities (e.g., the COVID-19 lockdown).

DOI： 10.5194/acp-21-5965-2021

Web of Science

Scopus

記述言語：英語   掲載種別：研究論文（学術雑誌）   出版者・発行元：Proceedings of the National Academy of Sciences of the United States of America  

Plastic pollution is one of the most pressing environmental and social issues of the 21st century. Recent work has highlighted the atmosphere's role in transporting microplastics to remote locations [S. Allen et al., Nat. Geosci. 12, 339 (2019) and J. Brahney, M. Hallerud, E. Heim, M. Hahnenberger, S. Sukumaran, Science 368, 1257-1260 (2020)]. Here, we use in situ observations of microplastic deposition combined with an atmospheric transport model and optimal estimation techniques to test hypotheses of the most likely sources of atmospheric plastic. Results suggest that atmospheric microplastics in the western United States are primarily derived from secondary re-emission sources including roads (84%), the ocean (11%), and agricultural soil dust (5%). Using our best estimate of plastic sources and modeled transport pathways, most continents were net importers of plastics from the marine environment, underscoring the cumulative role of legacy pollution in the atmospheric burden of plastic. This effort uses high-resolution spatial and temporal deposition data along with several hypothesized emission sources to constrain atmospheric plastic. Akin to global biogeochemical cycles, plastics now spiral around the globe with distinct atmospheric, oceanic, cryospheric, and terrestrial residence times. Though advancements have been made in the manufacture of biodegradable polymers, our data suggest that extant nonbiodegradable polymers will continue to cycle through the earth's systems. Due to limited observations and understanding of the source processes, there remain large uncertainties in the transport, deposition, and source attribution of microplastics. Thus, we prioritize future research directions for understanding the plastic cycle.

DOI： 10.1073/pnas.2020719118

Web of Science

Scopus

PubMed

記述言語：英語   掲載種別：研究論文（学術雑誌）   出版者・発行元：npj Climate and Atmospheric Science  

Anthropogenic iron oxide aerosols (FeOx) have been identified as a climatically significant atmospheric light absorber, and as a contributor of free iron to the oceans. Here we provide global-scale constraints on their atmospheric abundance with measurements over the remote Pacific and Atlantic Oceans from aircraft campaigns spanning 10 years. We find FeOx-like aerosols are transported far from source regions with similar efficiency as black carbon particles. Strong contrast in concentrations was observed between the Northern and Southern Hemisphere Pacific. We provide observational constraints in remote regions on the ambient ratios of FeOx relative to BC from fossil fuel burning. Comparison with a global aerosol model tuned to recent observations in East-Asian source regions confirm an upward revision of emissions based on model/observation comparison over the Pacific receptor region. We find that anthropogenic FeOx-like particles generate global-scale shortwave atmospheric heating 0.3–26% of that of black carbon in remote regions where concentrations of both aerosols are very low.

DOI： 10.1038/s41612-021-00171-0

Web of Science

Scopus

記述言語：英語   掲載種別：研究論文（学術雑誌）   出版者・発行元：Polar Science  

Aerosols and clouds play important roles in the Arctic climate. Conversely, aerosol emissions and cloud formation are affected by changes in the Arctic climate. This paper reviews studies of aerosols and clouds performed during the Arctic Challenge for Sustainability (ArCS) project carried out by the National Institute of Polar Research (NIPR) in Japan and collaborating institutions. The ArCS project included intensive studies of black carbon aerosols (BC). We installed Continuous Soot Monitoring System (COSMOS) instruments to measure atmospheric BC at four locations in the Arctic, establishing the Arctic BC COSMOS Measurement Network (ABCM-net). We also measured BC concentrations in snowpack in extensive areas of the Arctic and showed that previous studies have greatly overestimated BC in snowpack. We developed and improved new aerosol models that achieved better agreements with measurements of BC in the Arctic atmosphere, snowpack, and falling snow. We made new estimates of radiative forcing of BC in the Arctic atmosphere and snow/ice surfaces that lower their albedo. In addition to these researches on BC, we made accurate measurements of ice nucleating particles (INPs) at Ny-Ålesund, Svalbard, showing that their concentrations increased in summer as a result of dust particle emissions from glacial outwash sediments. This high ice nucleating ability was likely due to the presence of organic substances mixed with the dust particles. We also made continuous cloud radar measurements and the first continuous in-situ measurements of cloud microphysical properties in the Arctic at Ny-Ålesund. Results from these cloud measurements and their relationship with aerosols are described.

DOI： 10.1016/j.polar.2020.100621

Web of Science

Scopus

担当区分：最終著者,　責任著者   記述言語：英語   掲載種別：研究論文（学術雑誌）   出版者・発行元：Journal of Geophysical Research: Atmospheres  

In-cloud wet scavenging dominates the wet removal of aerosols in the atmosphere, but is not well represented in climate models. Aircraft measurements of black carbon (BC) concentrations suggest that models commonly overestimate BC concentrations in the upper troposphere of the tropics by more than one order of magnitude but underestimate BC burdens in polar latitudes. In this study, we improved the in-cloud wet scavenging parameterizations for convective clouds and mixed-phase clouds to better characterize BC abundances in the remote atmosphere (remote oceans and polar regions) with a global model, CAM5-ATRAS2. The modified wet scavenging processes in the model achieved a more realistic simulation of BC concentrations over both the tropics and the Arctic. The new, unified scheme for vertical transport and wet removal during deep convection generally reproduced the observed low mixing ratios (about 0.1 ng kg−1) of BC in the middle and upper troposphere over the tropics, and the Wegener–Bergeron–Findeisen process (WBF) lowered the wet removal efficiency of BC from mixed-phase clouds and consequently increased BC burdens in the Arctic by about a factor of 2. The BC direct radiative forcings increased by 20% globally (from 0.26 to 0.31 W m−2), and more importantly by a factor of 2 in the Arctic (from 0.09 to 0.18 W m−2). Our results indicated that good agreement between modeled and observed BC concentrations could be obtained in the remote atmosphere without requiring the relatively short global BC lifetime (∼4 days) suggested by previous studies.

DOI： 10.1029/2020JD033890

Web of Science

Scopus

記述言語：英語   掲載種別：研究論文（学術雑誌）  

記述言語：英語   掲載種別：研究論文（学術雑誌）   出版者・発行元：Atmospheric Chemistry and Physics  

Within the framework of the AeroCom (Aerosol Comparisons between Observations and Models) initiative, the state-of-the-art modelling of aerosol optical properties is assessed from 14 global models participating in the phase III control experiment (AP3). The models are similar to CMIP6/AerChemMIP Earth System Models (ESMs) and provide a robust multi-model ensemble. Inter-model spread of aerosol species lifetimes and emissions appears to be similar to that of mass extinction coefficients (MECs), suggesting that aerosol optical depth (AOD) uncertainties are associated with a broad spectrum of parameterised aerosol processes. Total AOD is approximately the same as in AeroCom phase I (AP1) simulations. However, we find a 50 % decrease in the optical depth (OD) of black carbon (BC), attributable to a combination of decreased emissions and lifetimes. Relative contributions from sea salt (SS) and dust (DU) have shifted from being approximately equal in AP1 to SS contributing about 2/3 of the natural AOD in AP3. This shift is linked with a decrease in DU mass burden, a lower DU MEC, and a slight decrease in DU lifetime, suggesting coarser DU particle sizes in AP3 compared to AP1. Relative to observations, the AP3 ensemble median and most of the participating models underestimate all aerosol optical properties investigated, that is, total AOD as well as fine and coarse AOD (AODf, AODc), Ångström exponent (AE), dry surface scattering (SCdry), and absorption (ACdry) coefficients. Compared to AERONET, the models underestimate total AOD by ca. 21 % ± 20 % (as inferred from the ensemble median and interquartile range). Against satellite data, the ensemble AOD biases range from -37 % (MODIS-Terra) to -16 % (MERGED-FMI, a multi-satellite AOD product), which we explain by differences between individual satellites and AERONET measurements themselves. Correlation coefficients (R) between model and observation AOD records are generally high (R>0.75), suggesting that the models are capable of capturing spatio-temporal variations in AOD. We find a much larger underestimate in coarse AODc (∼ -45 % ± 25 %) than in fine AODf (∼ -15 % ± 25 %) with slightly increased inter-model spread compared to total AOD. These results indicate problems in the modelling of DU and SS. The AODc bias is likely due to missing DU over continental land masses (particularly over the United States, SE Asia, and S. America), while marine AERONET sites and the AATSR SU satellite data suggest more moderate oceanic biases in AODc. Column AEs are underestimated by about 10 % ± 16 %. For situations in which measurements show AE > 2, models underestimate AERONET AE by ca. 35 %. In contrast, all models (but one) exhibit large overestimates in AE when coarse aerosol dominates (bias ca. +140 % if observed AE < 0.5). Simulated AE does not span the observed AE variability. These results indicate that models overestimate particle size (or underestimate the fine-mode fraction) for fine-dominated aerosol and underestimate size (or overestimate the fine-mode fraction) for coarse-dominated aerosol. This must have implications for lifetime, water uptake, scattering enhancement, and the aerosol radiative effect, which we can not quantify at this moment. Comparison against Global Atmosphere Watch (GAW) in situ data results in mean bias and inter-model variations of -35 % ± 25 % and -20 % ± 18 % for SCdry and ACdry, respectively. The larger underestimate of SCdry than ACdry suggests the models will simulate an aerosol single scattering albedo that is too low. The larger underestimate of SCdry than ambient air AOD is consistent with recent findings that models overestimate scattering enhancement due to hygroscopic growth. The broadly consistent negative bias in AOD and surface scattering suggests an underestimate of aerosol radiative effects in current global aerosol models. Considerable inter-model diversity in the simulated optical properties is often found in regions that are, unfortunately, not or only sparsely covered by ground-based observations. This includes, for instance, the Sahara, Amazonia, central Australia, and the South Pacific. This highlights the need for a better site coverage in the observations, which would enable us to better assess the models, but also the performance of satellite products in these regions. Using fine-mode AOD as a proxy for present-day aerosol forcing estimates, our results suggest that models underestimate aerosol forcing by ca. -15 %, however, with a considerably large interquartile range, suggesting a spread between -35 % and +10 %.

DOI： 10.5194/acp-21-87-2021

Web of Science

Scopus

担当区分：責任著者   記述言語：英語   掲載種別：研究論文（学術雑誌）   出版者・発行元：Scientific Online Letters on the Atmosphere  

The emission of Asian dust in arid regions of East Asia is controlled by many land surface parameters such as snow cover, soil moisture, and vegetation. In climate models, these factors are represented by the threshold friction velocity u*t, but its treatment has large uncertainties. Here we show that the treatment of u*tis important for estimating the emissions, transport, and climate impacts of Asian dust. Our global aerosol model simulates dust event frequencies that better agree with observations in East Asia when u*t over a smooth surface is changed from the default value of 0.23 m s−1 to an observation-based value of 0.40 m s−1. Also, seasonal Asian dust emissions become more variable, increasing by 31% in spring and decreasing by 46% in summer and fall, and the annual amounts of Asian dust transported and deposited over the North Pacific (Arctic) increase by 43% and 49% (130% and 73%), respectively. Our results demonstrate that better representation of u*t in climate models is necessary to improve estimates of the emissions and transport of Asian dust and better understand its roles in the Earth system, such as its interactions with radiation, clouds, snow/ice albedo, and land and ocean biogeochemistry.

DOI： 10.2151/sola.2021-042

Web of Science

Scopus

CiNii Research

担当区分：最終著者   記述言語：英語   掲載種別：研究論文（学術雑誌）   出版者・発行元：One Earth  

Black carbon (BC) particles, also known as soot, deteriorate air quality and threaten public health. BC is emitted from the incomplete combustion of fossil fuel, which is a major energy source in the world today. Therefore, evaluating the impact of BC on global public health is vital, especially in the context of growing global population and energy demand. Since the atmospheric lifetime and deposition efficiency of BC after inhalation are governed by the size and chemical composition, realistic representation of those properties in models is required for such evaluation, yet is currently lacking. Here, we show that a simple but commonly found representation of size and chemical composition of BC particles in global models results in globally prevalent underestimation of the respiratory deposited BC mass concentration. The results emphasize that realistic representation of BC particles is indispensable to the evaluation and hence the mitigation of BC impacts on global public health. Black carbon (BC) particles deteriorate air quality and threaten public health. BC is emitted from the incomplete combustions of fossil fuels. Our world relies heavily on fossil fuels for energy and has rising population and energy demand, therefore, it is imperative to evaluate the impact of BC on global public health. Here, we show that a common and simple representation of BC particles in global climate models causes globally prevalent underestimation of respiratory deposited BC mass concentration. Also, the uncertainty of the sizes of BC particles at emission is shown to modulate the underestimation. The results highlight the need of a more realistic representation of BC, which is currently lacking, in order to better assess the public health impact. Multidisciplinary studies involving atmospheric science, epidemiology, and toxicology can establish a scientific foundation for BC mitigation policy, which benefits the sustainable development of an increasingly urban world. Black carbon (BC) particles are emitted from the incomplete combustions of fossil fuels and deteriorate air quality and threaten public health. Evaluating the impact of BC on global public health is challenging and requires realistic aerosol representation in models, which is currently lacking. We find that simple aerosol representations in global climate models lead to globally prevalent underestimation of respiratory deposited mass concentration of BC. Besides, the uncertainties in BC emission size distributions modulate the magnitude of the underestimation.

DOI： 10.1016/j.oneear.2020.11.004

Web of Science

Scopus

記述言語：英語   掲載種別：研究論文（学術雑誌）   出版者・発行元：Journal of Geophysical Research: Atmospheres  

Ice nucleating particles (INPs) originating from Asia are expected to have large impacts on aerosol-cloud-precipitation interactions on local, regional, and global scales. However, their seasonal variability is poorly understood. Here, we present a year-round record of atmospheric INPs measured on Tokyo Skytree, which is the world's tallest broadcasting tower located in the Tokyo Metropolitan area. The INP number concentrations showed relatively small variations in the temperature regime below −20°C, whereas the values were episodically enhanced by long-range transported Asian dusts. On the other hand, the INP spectra in the temperature regime warmer than −20°C exhibited measurable seasonal variations. Notably, the INP number concentrations in the temperature regime between −15°C and −10°C tended to indicate higher values in warm/wet seasons and lower values in cold/dry seasons. Our results suggest that Asian dust events and seasonal variations in certain particles of biological origin linked to local/regional meteorology might influence the seasonal trends of the INP spectra over the Tokyo Metropolitan area.

DOI： 10.1029/2020JD033658

Web of Science

Scopus

担当区分：筆頭著者,　最終著者,　責任著者   記述言語：英語   掲載種別：研究論文（学術雑誌）   出版者・発行元：Journal of Geophysical Research: Atmospheres  

The positive radiative forcing of black carbon (BC) aerosol depends not only on the spatial and temporal distribution of BC but also its absorption efficiency. The mass absorption cross section (MAC) of BC is enhanced by atmospheric aging processes that increase particle size and non-BC coating amounts (mixing state) of BC-containing particles. However, the representation of MAC (or absorption enhancement) in current global aerosol models has a large uncertainty. This study used a global aerosol model that resolves particle size and mixing state to show that the MAC of anthropogenic BC has increased by 50% from preindustrial to present-day conditions (from 5.6 to 8.6 m2 g−1) because faster present-day aging processes increase the fraction of thickly coated BC particles, which have high absorption efficiency. This effect is apparent only when the model considers BC mixing state with sufficient resolution. The impact of this MAC enhancement on BC direct radiative forcing is estimated to be 0.051–0.086 W m−2 globally (22–37% of anthropogenic BC direct radiative forcing, 0.23 W m−2) and exceeds 0.5 W m−2 near-source regions in East Asia. Sensitivity simulations show that BC direct radiative forcing and MAC are highly sensitive to non-BC emissions, secondary aerosol formation, and aerosol size distribution and mixing state in emissions. We must therefore improve our understanding of these factors by further observations and reduce their discrepancies between models to achieve better estimates of BC absorption efficiency and radiative forcing.

DOI： 10.1029/2019JD032316

Web of Science

Scopus

記述言語：英語   掲載種別：研究論文（学術雑誌）   出版者・発行元：Geophysical Research Letters  

The iron cycle is a key component of the Earth system. Yet how variable the atmospheric flux of soluble (bioaccessible) iron into oceans is, and how this variability is modulated by human activity and a changing climate, is not well known. For the first time, we characterize Satellite Era (1980 to 2015) daily-to-interannual modeled soluble iron emission and deposition variability from both pyrogenic (fires and anthropogenic combustion) and dust sources. Statistically significant emission trends exist: dust iron decreases, fire iron slightly increases, and anthropogenic iron increases. A strong temporal variability in deposition to ocean basins is found, and, for most regions, dust iron dominates the absolute deposition magnitude, fire iron is an important contributor to temporal variability, and anthropogenic iron imposes a significant increasing trend. Quantifying soluble iron daily-to-interannual deposition variability from all major iron sources, not only dust, will advance quantification of changes in marine biogeochemistry in response to the continuing human perturbation to the Earth System.

DOI： 10.1029/2020GL089688

Web of Science

Scopus

記述言語：英語   掲載種別：研究論文（学術雑誌）   出版者・発行元：Atmospheric Chemistry and Physics  

The uptake of water by atmospheric aerosols has a pronounced effect on particle light scattering properties, which in turn are strongly dependent on the ambient relative humidity (RH). Earth system models need to account for the aerosol water uptake and its influence on light scattering in order to properly capture the overall radiative effects of aerosols. Here we present a comprehensive model measurement evaluation of the particle light scattering enhancement factor f (RH), defined as the particle light scattering coefficient at elevated RH (here set to 85 %) divided by its dry value. The comparison uses simulations from 10 Earth system models and a global dataset of surface-based in situ measurements. In general, we find a large diversity in the magnitude of predicted f (RH) amongst the different models, which can not be explained by the site types. Based on our evaluation of sea salt scattering enhancement and simulated organic mass fraction, there is a strong indication that differences in the model parameterizations of hygroscopicity and model chemistry are driving at least some of the observed diversity in simulated f (RH). Additionally, a key point is that defining dry conditions is difficult from an observational point of view and, depending on the aerosol, may influence the measured f (RH). The definition of dry also impacts our model evaluation, because several models exhibit significant water uptake between RH D0% and 40 %. The multisite average ratio between model outputs and measurements is 1.64 when RHD0% is assumed as the model dry RH and 1.16 when RHD40% is the model dry RH value. The overestimation by the models is believed to originate from the hygroscopicity parameterizations at the lower RH range which may not implement all phenomena taking place (i.e., not fully dried particles and hysteresis effects). This will be particularly relevant when a location is dominated by a deliquescent aerosol such as sea salt. Our results emphasize the need to consider the measurement conditions in such comparisons and recognize that measurements referred to as dry may not be dry in model terms. Recommendations for future model measurement evaluation and model improvements are provided.

DOI： 10.5194/acp-20-10231-2020

Web of Science

Scopus

担当区分：筆頭著者,　責任著者   記述言語：英語   掲載種別：研究論文（学術雑誌）   出版者・発行元：Geophysical Research Letters  

The representation of aerosol activation into cloud droplets in climate models is important for accurate understanding of aerosol radiative impacts on the Arctic climate, but it remains highly uncertain. Here we show that the uncertainty range of subgrid vertical velocity (SVV) and maximum supersaturation (SSmax) in aerosol activation produces fourfold to fivefold differences in the direct radiative effect of black carbon (BC) in the Arctic (0.091–0.40 W m−2) because SVV and SSmax determine the activated fraction and wet removal efficiency of aerosols. Aerosols are particularly sensitive to SVV in remote regions but not near their sources because many aerosols near sources are not yet influenced by wet removal processes. Our results demonstrate that SVV treatment is a major source of uncertainty in Arctic aerosol simulations and may be key for reducing the large discrepancies among global models in estimates of BC and its radiative effects in the Arctic.

DOI： 10.1029/2020GL088978

Web of Science

Scopus

記述言語：英語   掲載種別：研究論文（学術雑誌）   出版者・発行元：Journal of Geophysical Research: Atmospheres  

Black carbon (BC) aerosol deposited in and onto Arctic snow increases the snow's absorption of sunlight and accelerates snowmelt. Wet removal of BC from the atmosphere plays a key role in determining its abundance in the Arctic atmosphere and in Arctic snow. However, this process is poorly understood, mainly due to the scarcity of relevant measurements. To study wet deposition of BC, we made measurements of mass concentration of BC in snow and rain (CMBC) and of BC in air (MBC) with high accuracy (16% and 10%, respectively) at the Barrow Atmospheric Baseline Observatory, Alaska, from July 2013 to August 2017 and analyzed them along with routinely measured meteorological parameters from Barrow. Monthly mean MBC near the surface and CMBC were poorly correlated from midwinter to early spring, when CMBC was close to the annual median while MBC was at its annual peak. Seasonal variations in the altitude distribution of MBC may lead to these differences in seasonal variation of MBC near the surface and CMBC. About 50% of the annual wet deposition of BC occurred in the 3 months of summer, associated with high values of total precipitation and BC originating from biomass burning. Size distributions of BC in snow and rain were stable throughout the year, suggesting that the size distribution of BC in the lower troposphere was similarly stable. Calculations by two global models reproduced the observed seasonal variations of CMBC and showed that BC from biomass burning dominated CMBC in summer.

DOI： 10.1029/2019JD032240

Web of Science

Scopus

記述言語：英語   掲載種別：研究論文（学術雑誌）   出版者・発行元：Journal of Geophysical Research: Atmospheres  

Black carbon (BC), brown carbon, and light-absorbing iron oxides (FeOx) aerosols affect Earth's energy budget through their strong absorption of solar radiation. FeOx aerosols can also affect global biogeochemical cycles through their role as a nutrient for oceanic phytoplankton. However, observational data for these aerosols required for evaluating their effects using global models are scarce, especially for FeOx. Here, we summarize and compare the data sets of BC and FeOx from five ground-based and three aircraft observation campaigns conducted in the East Asian and Arctic regions during the 2009–2018 period acquired using a modified single-particle soot photometer. In these campaigns, >80% of FeOx-containing aerosols in the 170–270 nm FeOx core size range had microphysical features indicating an anthropogenic origin. The particle size distribution for each of the BC and FeOx was similar in all of the data sets except for those dominated by fresh urban pollution or pristine Arctic air. The campaign-averaged mass concentrations of FeOx and BC were ~60–360 ng/m3 and ~240–1,300 ng/m3, respectively, in East Asia, and ~6 ng/m3 and ~20–30 ng/m3, respectively, in the Arctic. The campaign-averaged FeOx/BC mass concentration ratio varied within a narrow range of 0.2–0.6 in both East Asian and Arctic regions. In every campaign, FeOx, BC, and carbon monoxide were tightly correlated with each other with similar slope to the urban campaigns (around Tokyo), implying the spatiotemporal variation of anthropogenic FeOx emission around northern middle-to-high latitudes is similar to those of anthropogenic BC and CO emissions.

DOI： 10.1029/2019JD032301

Web of Science

Scopus

記述言語：日本語   掲載種別：研究論文（学術雑誌）  

記述言語：英語   掲載種別：研究論文（学術雑誌）   出版者・発行元：Atmospheric Chemistry and Physics  

A total of 16 global chemistry transport models and general circulation models have participated in this study; 14 models have been evaluated with regard to their ability to reproduce the near-surface observed number concentration of aerosol particles and cloud condensation nuclei (CCN), as well as derived cloud droplet number concentration (CDNC). Model results for the period 2011-2015 are compared with aerosol measurements (aerosol particle number, CCN and aerosol particle composition in the submicron fraction) from nine surface stations located in Europe and Japan. The evaluation focuses on the ability of models to simulate the average across time state in diverse environments and on the seasonal and short-term variability in the aerosol properties. There is no single model that systematically performs best across all environments represented by the observations. Models tend to underestimate the observed aerosol particle and CCN number concentrations, with average normalized mean bias (NMB) of all models and for all stations, where data are available, of -24% and -35% for particles with dry diameters >50 and >120nm, as well as -36% and -34% for CCN at supersaturations of 0.2% and 1.0%, respectively. However, they seem to behave differently for particles activating at very low supersaturations (<0.1%) than at higher ones. A total of 15 models have been used to produce ensemble annual median distributions of relevant parameters. The model diversity (defined as the ratio of standard deviation to mean) is up to about 3 for simulated N3 (number concentration of particles with dry diameters larger than 3nm) and up to about 1 for simulated CCN in the extra-polar regions. A global mean reduction of a factor of about 2 is found in the model diversity for CCN at a supersaturation of 0.2% (CCN0.2) compared to that for N3, maximizing over regions where new particle formation is important. An additional model has been used to investigate potential causes of model diversity in CCN and bias compared to the observations by performing a perturbed parameter ensemble (PPE) accounting for uncertainties in 26 aerosol-related model input parameters. This PPE suggests that biogenic secondary organic aerosol formation and the hygroscopic properties of the organic material are likely to be the major sources of CCN uncertainty in summer, with dry deposition and cloud processing being dominant in winter. Models capture the relative amplitude of the seasonal variability of the aerosol particle number concentration for all studied particle sizes with available observations (dry diameters larger than 50, 80 and 120nm). The short-term persistence time (on the order of a few days) of CCN concentrations, which is a measure of aerosol dynamic behavior in the models, is underestimated on average by the models by 40% during winter and 20% in summer. In contrast to the large spread in simulated aerosol particle and CCN number concentrations, the CDNC derived from simulated CCN spectra is less diverse and in better agreement with CDNC estimates consistently derived from the observations (average NMB -13% and -22% for updraft velocities 0.3 and 0.6ms-1, respectively). In addition, simulated CDNC is in slightly better agreement with observationally derived values at lower than at higher updraft velocities (index of agreement 0.64 vs. 0.65). The reduced spread of CDNC compared to that of CCN is attributed to the sublinear response of CDNC to aerosol particle number variations and the negative correlation between the sensitivities of CDNC to aerosol particle number concentration (Nd=Na) and to updraft velocity (Nd=w). Overall, we find that while CCN is controlled by both aerosol particle number and composition, CDNC is sensitive to CCN at low and moderate CCN concentrations and to the updraft velocity when CCN levels are high. Discrepancies are found in sensitivities Nd=Na and Nd=w; models may be predisposed to be too "aerosol sensitive" or "aerosol insensitive" in aerosol-cloud-climate interaction studies, even if they may capture average droplet numbers well. This is a subtle but profound finding that only the sensitivities can clearly reveal and may explain intermodel biases on the aerosol indirect effect.

DOI： 10.5194/acp-19-8591-2019

Web of Science

Scopus

PubMed

記述言語：英語   掲載種別：研究論文（学術雑誌）   出版者・発行元：npj Climate and Atmospheric Science  

Quantitative simulation of an aerosol’s lifecycle by regional-scale and global-scale atmospheric models is mandatory for unbiased analysis and prediction of aerosol radiative forcing and climate change. Globally, aerosol deposition is dominated by the rainout process, which is mostly triggered by activation of aerosols to liquid droplets in supersaturated domains of precipitating clouds. However, the actual environmental supersaturation value that aerosols experience in precipitating clouds is difficult for models to predict, and it has never been constrained by observations; as a result, there is large uncertainty in atmospheric aerosol simulations. Here, by a particle-tracer analysis of 37 rainfall events in East Asia, near the largest source region of anthropogenic aerosols in the northern hemisphere, we observed that the environmental supersaturation actually experienced by the removed aerosols in precipitating clouds averaged 0.08 ± 0.03% and ranged from 0.03 to 0.2%. Simulations by a mixing-state-resolved global aerosol model showed that the simulated long-range transport efficiency and global atmospheric burden of black carbon aerosols can be changed by a factor of two or three as a result of a change in the environmental supersaturation in precipitating clouds within just 0.08 ± 0.03%. This result is attributable to the fact that the sensitivity of an aerosol’s rainout efficiency to environmental supersaturation is higher for the less-aged black carbon concentrated near source regions. Our results suggest that observational constraints of environmental supersaturation in precipitating clouds, particularly near source regions, are of fundamental importance for accurate simulation of the atmospheric burden of black carbon and other aerosols.

DOI： 10.1038/s41612-019-0063-y

Web of Science

Scopus

記述言語：英語   掲載種別：研究論文（学術雑誌）   出版者・発行元：Aerosol and Air Quality Research  

New particle formation (NPF) from nucleation and subsequent nuclei growth, which is frequently observed in the troposphere, is critical to aerosol-cloud interactions yet difficult to simulate. In this work, regional simulations with the fully coupled NPF-explicit WRF-Chem model link NPF to cloud properties and to changes in both meteorology and air quality in the U.S. Midwest during summer 2008. Simulations that include NPF have higher concentrations of condensation nuclei, as anticipated from the particle production associated with nucleation, leading to enhanced concentrations of cloud condensation nuclei (CCN) at high supersaturations. However, the online-coupled model develops a number of unexpected features that can be traced to a feedback loop involving aqueous (in-cloud) oxidation of sulfur combined with boundary layer NPF. Simulations with NPF (relative to simulations without) exhibit reduced PM2.5 sulfate mass, cloud dimming (reductions in the cloud frequency, CCN concentration at a low supersaturation, cloud optical depth, and cloud droplet number concentration), and enhanced surface-reaching shortwave radiation. This effect of NPF on the PM2.5 mass is mostly absent for other constituents of PM2.5. The implications of this feedback loop, which is not considered in most climate and air quality modeling, are discussed.

DOI： 10.4209/aaqr.2018.05.0163

Web of Science

Scopus

記述言語：英語   掲載種別：研究論文（学術雑誌）  

CiNii Research

担当区分：筆頭著者,　責任著者   記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1038/s41467-018-05635-1

Web of Science

PubMed

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： doi:10.1038/s41612-018-0019-7

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1029/2017MS001219

Web of Science

Scopus

担当区分：筆頭著者,　責任著者   記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1038/s41467-018-03997-0

記述言語：英語   掲載種別：研究論文（学術雑誌）   出版者・発行元：Springer Nature  

New particle formation (NPF), nucleation of condensable vapors to the solid or liquid phase, contributes significantly to atmospheric aerosol particle number concentrations. With sufficient growth, these nucleated particles may be a significant source of cloud condensation nuclei (CCN), thus altering cloud albedo, structure, and lifetimes, and insolation reaching the Earth’s surface. Herein we present one of the first numerical experiments conducted at sufficiently high resolution and fidelity to quantify the impact of NPF on cloud radiative properties. Consistent with observations in spring over the Midwestern USA, NPF occurs frequently and on regional scales. However, NPF is not associated with enhancement of regional cloud albedo. These simulations indicate that NPF reduces ambient sulfuric acid concentrations sufficiently to inhibit growth of preexisting particles to CCN sizes, reduces CCN-sized particle concentrations, and reduces cloud albedo. The reduction in cloud albedo on NPF days results in a domain average positive top of atmosphere cloud radiative forcing, and thus warming, of 10 W m−2 and up to ~50 W m−2 in individual grid cells relative to a simulation in which NPF is excluded.

DOI： 10.1038/s41612-018-0019-7

Web of Science

Scopus

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.4209/aaqr.2016.12.0573

Web of Science

担当区分：筆頭著者,　最終著者,　責任著者   記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1002/2017MS000936

Web of Science

Scopus

担当区分：筆頭著者,　責任著者   記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1002/2017MS000937

Web of Science

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1002/2015JD024671

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1002/2015JD023998

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1002/2015JD023999

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.5194/acp-15-12283-2015

記述言語：日本語  

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1002/2014JD021693

Web of Science

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.5194/acp-14-11011-2014

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.5194/acp-14-10315-2014

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.5194/acp-14-9513-2014

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1002/2014JD022103

記述言語：日本語   掲載種別：研究論文（学術雑誌）  

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1002/2013JD020163

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1002/2013JD020262

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1002/jgrd.50821

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1002/jgrd.50702

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1002/jgrd.50317

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1029/2012JD018446

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1029/2011JD017324

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1029/2012GL052034

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1016/j.atmosenv.2012.02.080

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1029/2011JD016552

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1029/2011JD015830

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1029/2011JD016189

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1029/2011JD016025

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1029/2010JD015152

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1029/2010JD015067

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1029/2010JD013895

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.2151/jmsj.2010-401

Web of Science

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1029/2008JD010906

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1029/2008JD010164

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1029/2005JD006643