Articles | Volume 14, issue 22
Atmos. Chem. Phys., 14, 12455–12464, 2014
https://doi.org/10.5194/acp-14-12455-2014
© Author(s) 2014. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Atmos. Chem. Phys., 14, 12455–12464, 2014
https://doi.org/10.5194/acp-14-12455-2014
© Author(s) 2014. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
27 Nov 2014
Research article
| 27 Nov 2014
Modeling of gaseous methylamines in the global atmosphere: impacts of oxidation and aerosol uptake
F. Yu and G. Luo
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Particle number concentrations and size distributions in the stratosphere are studied through model simulations and comparisons with measurements. The nucleation scheme used in most of the solar geoengineering modeling studies over-predicts the nucleation rates and particle number concentrations in the stratosphere. The model based on updated nucleation schemes captures reasonably well some aspects of particle size distributions but misses some features. The possible reasons are discussed.
Katherine R. Travis, James H. Crawford, Gao Chen, Carolyn E. Jordan, Benjamin A. Nault, Hwajin Kim, Jose L. Jimenez, Pedro Campuzano-Jost, Jack E. Dibb, Jung-Hun Woo, Younha Kim, Shixian Zhai, Xuan Wang, Erin E. McDuffie, Gan Luo, Fangqun Yu, Saewung Kim, Isobel J. Simpson, Donald R. Blake, Limseok Chang, and Michelle J. Kim
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The 2016 Korea–United States Air Quality (KORUS-AQ) field campaign provided a unique set of observations to improve our understanding of PM2.5 pollution in South Korea. Models typically have errors in simulating PM2.5 in this region, which is of concern for the development of control measures. We use KORUS-AQ observations to improve our understanding of the mechanisms driving PM2.5 and the implications of model errors for determining PM2.5 that is attributable to local or foreign sources.
Noah S. Hirshorn, Lauren M. Zuromski, Christopher Rapp, Ian McCubbin, Fangqun Yu, and A. Gannet Hallar
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-338, https://doi.org/10.5194/acp-2022-338, 2022
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New particle formation (NPF) is a source of atmospheric aerosol number concentration that can impact climate by growing to larger sizes and under proper conditions, forming cloud condensation nuclei (CCN). Using novel methods, we find that at Storm Peak Laboratory, a remote mountaintop site in Colorado, NPF is observed to enhance CCN concentrations in the spring by a factor of 1.54 and in the winter by a factor of 1.36 which can occur on a regional scale having important climate implications.
Yanda Zhang, Fangqun Yu, Gan Luo, Jiwen Fan, and Shuai Liu
Atmos. Chem. Phys., 21, 17433–17451, https://doi.org/10.5194/acp-21-17433-2021, https://doi.org/10.5194/acp-21-17433-2021, 2021
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This paper explores the impacts of dust on summertime convective cloud and precipitation through a numerical experiment. The result indicates that the long-range-transported dust can notably affect the properties of convective cloud and precipitation by enhancing immersion freezing and invigorating convection. We also analyze the different dust effects predicted by the Morrison and SBM schemes, which are partially attributed to the saturation adjustment approach utilized in the bulk schemes.
Shixian Zhai, Daniel J. Jacob, Jared F. Brewer, Ke Li, Jonathan M. Moch, Jhoon Kim, Seoyoung Lee, Hyunkwang Lim, Hyun Chul Lee, Su Keun Kuk, Rokjin J. Park, Jaein I. Jeong, Xuan Wang, Pengfei Liu, Gan Luo, Fangqun Yu, Jun Meng, Randall V. Martin, Katherine R. Travis, Johnathan W. Hair, Bruce E. Anderson, Jack E. Dibb, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Jung-Hun Woo, Younha Kim, Qiang Zhang, and Hong Liao
Atmos. Chem. Phys., 21, 16775–16791, https://doi.org/10.5194/acp-21-16775-2021, https://doi.org/10.5194/acp-21-16775-2021, 2021
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Geostationary satellite aerosol optical depth (AOD) has tremendous potential for monitoring surface fine particulate matter (PM2.5). Our study explored the physical relationship between AOD and PM2.5 by integrating data from surface networks, aircraft, and satellites with the GEOS-Chem chemical transport model. We quantitatively showed that accurate simulation of aerosol size distributions, boundary layer depths, relative humidity, coarse particles, and diurnal variations in PM2.5 are essential.
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Emission controls were imposed in Beijing-Tianjin-Hebei in northern China in autumn-winter 2017. We find that regional PM2.5 targets (15 % decrease relative to previous year) were exceeded. Our analysis shows that decline in precursor emissions only leads to less than half (43 %) the improved air quality. Most of the change (57 %) is due to interannual variability in meteorology. Stricter emission controls may be necessary in years with unfavourable meteorology.
Xueshun Chen, Fangqun Yu, Wenyi Yang, Yele Sun, Huansheng Chen, Wei Du, Jian Zhao, Ying Wei, Lianfang Wei, Huiyun Du, Zhe Wang, Qizhong Wu, Jie Li, Junling An, and Zifa Wang
Atmos. Chem. Phys., 21, 9343–9366, https://doi.org/10.5194/acp-21-9343-2021, https://doi.org/10.5194/acp-21-9343-2021, 2021
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Atmospheric aerosol particles have significant climate and health effects that depend on aerosol size, composition, and mixing state. A new global-regional nested aerosol model with an advanced particle microphysics module and a volatility basis set organic aerosol module was developed to simulate aerosol microphysical processes. Simulations strongly suggest the important role of anthropogenic organic species in particle formation over the areas influenced by anthropogenic sources.
Xiaojing Shen, Junying Sun, Fangqun Yu, Ying Wang, Junting Zhong, Yangmei Zhang, Xinyao Hu, Can Xia, Sinan Zhang, and Xiaoye Zhang
Atmos. Chem. Phys., 21, 7039–7052, https://doi.org/10.5194/acp-21-7039-2021, https://doi.org/10.5194/acp-21-7039-2021, 2021
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In this work, we revealed the changes of PNSD and NPF events during the COVID-19 lockdown period in Beijing, China, to illustrate the impact of reduced primary emission and elavated atmospheric oxidized capicity on the nucleation and growth processes. The subsequent growth of nucleated particles and their contribution to the aerosol pollution formation were also explored, to highlight the necessity of controlling the nanoparticles in the future air quality management.
Ling Liu, Fangqun Yu, Kaipeng Tu, Zhi Yang, and Xiuhui Zhang
Atmos. Chem. Phys., 21, 6221–6230, https://doi.org/10.5194/acp-21-6221-2021, https://doi.org/10.5194/acp-21-6221-2021, 2021
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Trifluoroacetic acid (TFA) was previously proved to participate in sulfuric acid (SA)–dimethylamine (DMA) nucleation in Shanghai, China. However, complex atmospheric environments can influence the nucleation of aerosol significantly. We show the influence of different atmospheric conditions on the SA-DMA-TFA nucleation and find the enhancement by TFA can be significant in cold and polluted areas, which provides the perspective of the realistic role of TFA in different atmospheric environments.
Arshad Arjunan Nair and Fangqun Yu
Atmos. Chem. Phys., 20, 12853–12869, https://doi.org/10.5194/acp-20-12853-2020, https://doi.org/10.5194/acp-20-12853-2020, 2020
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Small particles in the atmosphere can affect cloud formation and properties and thus Earth's energy budget. These cloud condensation nuclei (CCN) contribute the largest uncertainties in climate change modeling. To reduce these uncertainties, it is important to quantify CCN numbers accurately, measurements of which are sparse. We propose and evaluate a machine learning method to estimate CCN, in the absence of their direct measurements, using more common measurements of weather and air quality.
Katherine R. Travis, Colette L. Heald, Hannah M. Allen, Eric C. Apel, Stephen R. Arnold, Donald R. Blake, William H. Brune, Xin Chen, Róisín Commane, John D. Crounse, Bruce C. Daube, Glenn S. Diskin, James W. Elkins, Mathew J. Evans, Samuel R. Hall, Eric J. Hintsa, Rebecca S. Hornbrook, Prasad S. Kasibhatla, Michelle J. Kim, Gan Luo, Kathryn McKain, Dylan B. Millet, Fred L. Moore, Jeffrey Peischl, Thomas B. Ryerson, Tomás Sherwen, Alexander B. Thames, Kirk Ullmann, Xuan Wang, Paul O. Wennberg, Glenn M. Wolfe, and Fangqun Yu
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Atmospheric models overestimate the rate of removal of trace gases by the hydroxyl radical (OH). This is a concern for studies of the climate and air quality impacts of human activities. Here, we evaluate the performance of a commonly used model of atmospheric chemistry against data from the NASA Atmospheric Tomography Mission (ATom) over the remote oceans where models have received little validation. The model is generally successful, suggesting that biases in OH may be a concern over land.
Gan Luo, Fangqun Yu, and Jonathan M. Moch
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This work improved pH calculation for cloud, rain, and wet surfaces, fraction of cloud available for aqueous-phase chemistry, rainout efficiencies for various types of cloud, empirical washout by rain and snow, and wet surface uptake in GEOS-Chem v12.6.0. We compared simulated mass concentrations of aerosol precursors and aerosols with surface monitoring networks, Arctic sites, and ATom observations, and showed that the model results with the updated wet processes agree better for most species.
Fangqun Yu, Alexey B. Nadykto, Gan Luo, and Jason Herb
Geosci. Model Dev., 13, 2663–2670, https://doi.org/10.5194/gmd-13-2663-2020, https://doi.org/10.5194/gmd-13-2663-2020, 2020
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Secondary particles formed via nucleation have important implications for air quality and climate. Here we describe nucleation rate lookup tables for four different nucleation mechanisms that can be readily used in chemistry transport and climate models. The nucleation rates predicted have been assessed against state-of-the-art laboratory measurements. The lookup tables cover a wide range of key parameters controlling binary, ternary, and ion-mediated nucleation in the Earth's atmosphere.
Fangqun Yu, Gan Luo, Arshad Arjunan Nair, James J. Schwab, James P. Sherman, and Yanda Zhang
Atmos. Chem. Phys., 20, 2591–2601, https://doi.org/10.5194/acp-20-2591-2020, https://doi.org/10.5194/acp-20-2591-2020, 2020
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Particle number concentration (PNC) is a key parameter important for the health and climate impacts of atmospheric aerosols. We show that, even during wintertime, regional nucleation occurs and contributes significantly to number concentrations of ultrafine particles and cloud condensation nuclei. Due to low biogenic emissions, wintertime regional nucleation is solely controlled by inorganic species, and ternary ion-mediated nucleation is able to capture the observed variations in PNC.
Xiaoyan Ma, Hailing Jia, Rong Tian, Fangqun Yu, and Jiagnan Li
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-54, https://doi.org/10.5194/acp-2020-54, 2020
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BC Mixing state, is one of critical microphysical properties to modulate optical properties, radiative forcing (RF), and climatic effect. However, it has been simply assumed previously as either external or internal mixing. In this study, by employing a nested GEOS-Chem-APM with predicted BC mixing state, we examined the effect of mixing state on aerosol optical properties, RF, and heating rate over East Asia. This will improve the predictions of aerosol climatic effect in the future.
Gan Luo, Fangqun Yu, and James Schwab
Geosci. Model Dev., 12, 3439–3447, https://doi.org/10.5194/gmd-12-3439-2019, https://doi.org/10.5194/gmd-12-3439-2019, 2019
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GEOS-Chem 12.0.0 has been recognized to significantly overestimate the concentrations of gaseous nitric acid, aerosol nitrate, and aerosol ammonium over the United States. In this study, we show that most or all of the overestimation issue appears to be associated with wet scavenging processes. With the updated wet scavenging scheme in this work, we successfully improve the skill of the model in predicting the three species concentrations, which are important for air quality and climate studies.
George S. Fanourgakis, Maria Kanakidou, Athanasios Nenes, Susanne E. Bauer, Tommi Bergman, Ken S. Carslaw, Alf Grini, Douglas S. Hamilton, Jill S. Johnson, Vlassis A. Karydis, Alf Kirkevåg, John K. Kodros, Ulrike Lohmann, Gan Luo, Risto Makkonen, Hitoshi Matsui, David Neubauer, Jeffrey R. Pierce, Julia Schmale, Philip Stier, Kostas Tsigaridis, Twan van Noije, Hailong Wang, Duncan Watson-Parris, Daniel M. Westervelt, Yang Yang, Masaru Yoshioka, Nikos Daskalakis, Stefano Decesari, Martin Gysel-Beer, Nikos Kalivitis, Xiaohong Liu, Natalie M. Mahowald, Stelios Myriokefalitakis, Roland Schrödner, Maria Sfakianaki, Alexandra P. Tsimpidi, Mingxuan Wu, and Fangqun Yu
Atmos. Chem. Phys., 19, 8591–8617, https://doi.org/10.5194/acp-19-8591-2019, https://doi.org/10.5194/acp-19-8591-2019, 2019
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Effects of aerosols on clouds are important for climate studies but are among the largest uncertainties in climate projections. This study evaluates the skill of global models to simulate aerosol, cloud condensation nuclei (CCN) and cloud droplet number concentrations (CDNCs). Model results show reduced spread in CDNC compared to CCN due to the negative correlation between the sensitivities of CDNC to aerosol number concentration (air pollution) and updraft velocity (atmospheric dynamics).
Fangqun Yu, Alexey B. Nadykto, Jason Herb, Gan Luo, Kirill M. Nazarenko, and Lyudmila A. Uvarova
Atmos. Chem. Phys., 18, 17451–17474, https://doi.org/10.5194/acp-18-17451-2018, https://doi.org/10.5194/acp-18-17451-2018, 2018
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Aerosol nucleation exerts important influences on the climate, hydrological cycle, and air quality. We have developed an advanced physical–chemical model that describes ion-induced and neutral nucleation involving ammonia, sulfuric acid, and water vapors. The model is shown to reproduce laboratory measurements taken under a wide range of conditions, offers physiochemical insights into the ternary nucleation process, and provides an accurate approach to calculate ternary rate in the atmosphere.
Jingbo Mao, Fangqun Yu, Yan Zhang, Jingyu An, Lin Wang, Jun Zheng, Lei Yao, Gan Luo, Weichun Ma, Qi Yu, Cheng Huang, Li Li, and Limin Chen
Atmos. Chem. Phys., 18, 7933–7950, https://doi.org/10.5194/acp-18-7933-2018, https://doi.org/10.5194/acp-18-7933-2018, 2018
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A few pptv of gaseous amines have been observed to affect particle nucleation and growth, and it is necessary to understand the sources and concentrations of atmospheric amines. This study presents the source-dependent amines to ammonia emission ratios and simulates methylamines concentrations in a polluted region in China with WRF-Chem. The performance of simulations based on source-dependent ratios is much better than those based on fixed ratios that have been assumed in all previous studies.
Maria Sand, Bjørn H. Samset, Yves Balkanski, Susanne Bauer, Nicolas Bellouin, Terje K. Berntsen, Huisheng Bian, Mian Chin, Thomas Diehl, Richard Easter, Steven J. Ghan, Trond Iversen, Alf Kirkevåg, Jean-François Lamarque, Guangxing Lin, Xiaohong Liu, Gan Luo, Gunnar Myhre, Twan van Noije, Joyce E. Penner, Michael Schulz, Øyvind Seland, Ragnhild B. Skeie, Philip Stier, Toshihiko Takemura, Kostas Tsigaridis, Fangqun Yu, Kai Zhang, and Hua Zhang
Atmos. Chem. Phys., 17, 12197–12218, https://doi.org/10.5194/acp-17-12197-2017, https://doi.org/10.5194/acp-17-12197-2017, 2017
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The role of aerosols in the changing polar climate is not well understood and the aerosols are poorly constrained in the models. In this study we have compared output from 16 different aerosol models with available observations at both poles. We show that the model median is representative of the observations, but the model spread is large. The Arctic direct aerosol radiative effect over the industrial area is positive during spring due to black carbon and negative during summer due to sulfate.
Fangqun Yu, Gan Luo, Alexey B. Nadykto, and Jason Herb
Atmos. Chem. Phys., 17, 4997–5005, https://doi.org/10.5194/acp-17-4997-2017, https://doi.org/10.5194/acp-17-4997-2017, 2017
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H2SO4–organics clustering thermodynamics from quantum studies has been employed to develop a scheme to include temperature dependence in an H2SO4–organics nucleation parameterization. We show that temperature has a strong impact on nucleation rates, particle number concentrations, and aerosol first indirect radiative forcing in summer. To our knowledge, the study represents the first attempt to study the temperature effect on organics-mediated nucleation in the global atmosphere.
F. Yu, G. Luo, S. C. Pryor, P. R. Pillai, S. H. Lee, J. Ortega, J. J. Schwab, A. G. Hallar, W. R. Leaitch, V. P. Aneja, J. N. Smith, J. T. Walker, O. Hogrefe, and K. L. Demerjian
Atmos. Chem. Phys., 15, 13993–14003, https://doi.org/10.5194/acp-15-13993-2015, https://doi.org/10.5194/acp-15-13993-2015, 2015
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The role of low-volatility organics in new particle formation (NPF) in the atmosphere is assessed. An empirical formulation in which formation rate is a function of the concentrations of sulfuric acid and low-volatility organics significantly overpredicts NPF in the summer.
Two different schemes predict quite different nucleation rates (including their spatial patterns), concentrations of cloud condensation nuclei, and aerosol first indirect radiative forcing in North America.
G. W. Mann, K. S. Carslaw, C. L. Reddington, K. J. Pringle, M. Schulz, A. Asmi, D. V. Spracklen, D. A. Ridley, M. T. Woodhouse, L. A. Lee, K. Zhang, S. J. Ghan, R. C. Easter, X. Liu, P. Stier, Y. H. Lee, P. J. Adams, H. Tost, J. Lelieveld, S. E. Bauer, K. Tsigaridis, T. P. C. van Noije, A. Strunk, E. Vignati, N. Bellouin, M. Dalvi, C. E. Johnson, T. Bergman, H. Kokkola, K. von Salzen, F. Yu, G. Luo, A. Petzold, J. Heintzenberg, A. Clarke, J. A. Ogren, J. Gras, U. Baltensperger, U. Kaminski, S. G. Jennings, C. D. O'Dowd, R. M. Harrison, D. C. S. Beddows, M. Kulmala, Y. Viisanen, V. Ulevicius, N. Mihalopoulos, V. Zdimal, M. Fiebig, H.-C. Hansson, E. Swietlicki, and J. S. Henzing
Atmos. Chem. Phys., 14, 4679–4713, https://doi.org/10.5194/acp-14-4679-2014, https://doi.org/10.5194/acp-14-4679-2014, 2014
X. Ma, K. Bartlett, K. Harmon, and F. Yu
Atmos. Meas. Tech., 6, 2391–2401, https://doi.org/10.5194/amt-6-2391-2013, https://doi.org/10.5194/amt-6-2391-2013, 2013
Fangqun Yu, Gan Luo, Arshad Arjunan Nair, Sebastian Eastham, Christina J. Williamson, Agnieszka Kupc, and Charles A. Brock
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-487, https://doi.org/10.5194/acp-2022-487, 2022
Preprint under review for ACP
Short summary
Short summary
Particle number concentrations and size distributions in the stratosphere are studied through model simulations and comparisons with measurements. The nucleation scheme used in most of the solar geoengineering modeling studies over-predicts the nucleation rates and particle number concentrations in the stratosphere. The model based on updated nucleation schemes captures reasonably well some aspects of particle size distributions but misses some features. The possible reasons are discussed.
Katherine R. Travis, James H. Crawford, Gao Chen, Carolyn E. Jordan, Benjamin A. Nault, Hwajin Kim, Jose L. Jimenez, Pedro Campuzano-Jost, Jack E. Dibb, Jung-Hun Woo, Younha Kim, Shixian Zhai, Xuan Wang, Erin E. McDuffie, Gan Luo, Fangqun Yu, Saewung Kim, Isobel J. Simpson, Donald R. Blake, Limseok Chang, and Michelle J. Kim
Atmos. Chem. Phys., 22, 7933–7958, https://doi.org/10.5194/acp-22-7933-2022, https://doi.org/10.5194/acp-22-7933-2022, 2022
Short summary
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The 2016 Korea–United States Air Quality (KORUS-AQ) field campaign provided a unique set of observations to improve our understanding of PM2.5 pollution in South Korea. Models typically have errors in simulating PM2.5 in this region, which is of concern for the development of control measures. We use KORUS-AQ observations to improve our understanding of the mechanisms driving PM2.5 and the implications of model errors for determining PM2.5 that is attributable to local or foreign sources.
Noah S. Hirshorn, Lauren M. Zuromski, Christopher Rapp, Ian McCubbin, Fangqun Yu, and A. Gannet Hallar
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-338, https://doi.org/10.5194/acp-2022-338, 2022
Preprint under review for ACP
Short summary
Short summary
New particle formation (NPF) is a source of atmospheric aerosol number concentration that can impact climate by growing to larger sizes and under proper conditions, forming cloud condensation nuclei (CCN). Using novel methods, we find that at Storm Peak Laboratory, a remote mountaintop site in Colorado, NPF is observed to enhance CCN concentrations in the spring by a factor of 1.54 and in the winter by a factor of 1.36 which can occur on a regional scale having important climate implications.
Yanda Zhang, Fangqun Yu, Gan Luo, Jiwen Fan, and Shuai Liu
Atmos. Chem. Phys., 21, 17433–17451, https://doi.org/10.5194/acp-21-17433-2021, https://doi.org/10.5194/acp-21-17433-2021, 2021
Short summary
Short summary
This paper explores the impacts of dust on summertime convective cloud and precipitation through a numerical experiment. The result indicates that the long-range-transported dust can notably affect the properties of convective cloud and precipitation by enhancing immersion freezing and invigorating convection. We also analyze the different dust effects predicted by the Morrison and SBM schemes, which are partially attributed to the saturation adjustment approach utilized in the bulk schemes.
Shixian Zhai, Daniel J. Jacob, Jared F. Brewer, Ke Li, Jonathan M. Moch, Jhoon Kim, Seoyoung Lee, Hyunkwang Lim, Hyun Chul Lee, Su Keun Kuk, Rokjin J. Park, Jaein I. Jeong, Xuan Wang, Pengfei Liu, Gan Luo, Fangqun Yu, Jun Meng, Randall V. Martin, Katherine R. Travis, Johnathan W. Hair, Bruce E. Anderson, Jack E. Dibb, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Jung-Hun Woo, Younha Kim, Qiang Zhang, and Hong Liao
Atmos. Chem. Phys., 21, 16775–16791, https://doi.org/10.5194/acp-21-16775-2021, https://doi.org/10.5194/acp-21-16775-2021, 2021
Short summary
Short summary
Geostationary satellite aerosol optical depth (AOD) has tremendous potential for monitoring surface fine particulate matter (PM2.5). Our study explored the physical relationship between AOD and PM2.5 by integrating data from surface networks, aircraft, and satellites with the GEOS-Chem chemical transport model. We quantitatively showed that accurate simulation of aerosol size distributions, boundary layer depths, relative humidity, coarse particles, and diurnal variations in PM2.5 are essential.
Gongda Lu, Eloise A. Marais, Tuan V. Vu, Jingsha Xu, Zongbo Shi, James D. Lee, Qiang Zhang, Lu Shen, Gan Luo, and Fangqun Yu
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-428, https://doi.org/10.5194/acp-2021-428, 2021
Revised manuscript not accepted
Short summary
Short summary
Emission controls were imposed in Beijing-Tianjin-Hebei in northern China in autumn-winter 2017. We find that regional PM2.5 targets (15 % decrease relative to previous year) were exceeded. Our analysis shows that decline in precursor emissions only leads to less than half (43 %) the improved air quality. Most of the change (57 %) is due to interannual variability in meteorology. Stricter emission controls may be necessary in years with unfavourable meteorology.
Xueshun Chen, Fangqun Yu, Wenyi Yang, Yele Sun, Huansheng Chen, Wei Du, Jian Zhao, Ying Wei, Lianfang Wei, Huiyun Du, Zhe Wang, Qizhong Wu, Jie Li, Junling An, and Zifa Wang
Atmos. Chem. Phys., 21, 9343–9366, https://doi.org/10.5194/acp-21-9343-2021, https://doi.org/10.5194/acp-21-9343-2021, 2021
Short summary
Short summary
Atmospheric aerosol particles have significant climate and health effects that depend on aerosol size, composition, and mixing state. A new global-regional nested aerosol model with an advanced particle microphysics module and a volatility basis set organic aerosol module was developed to simulate aerosol microphysical processes. Simulations strongly suggest the important role of anthropogenic organic species in particle formation over the areas influenced by anthropogenic sources.
Xiaojing Shen, Junying Sun, Fangqun Yu, Ying Wang, Junting Zhong, Yangmei Zhang, Xinyao Hu, Can Xia, Sinan Zhang, and Xiaoye Zhang
Atmos. Chem. Phys., 21, 7039–7052, https://doi.org/10.5194/acp-21-7039-2021, https://doi.org/10.5194/acp-21-7039-2021, 2021
Short summary
Short summary
In this work, we revealed the changes of PNSD and NPF events during the COVID-19 lockdown period in Beijing, China, to illustrate the impact of reduced primary emission and elavated atmospheric oxidized capicity on the nucleation and growth processes. The subsequent growth of nucleated particles and their contribution to the aerosol pollution formation were also explored, to highlight the necessity of controlling the nanoparticles in the future air quality management.
Ling Liu, Fangqun Yu, Kaipeng Tu, Zhi Yang, and Xiuhui Zhang
Atmos. Chem. Phys., 21, 6221–6230, https://doi.org/10.5194/acp-21-6221-2021, https://doi.org/10.5194/acp-21-6221-2021, 2021
Short summary
Short summary
Trifluoroacetic acid (TFA) was previously proved to participate in sulfuric acid (SA)–dimethylamine (DMA) nucleation in Shanghai, China. However, complex atmospheric environments can influence the nucleation of aerosol significantly. We show the influence of different atmospheric conditions on the SA-DMA-TFA nucleation and find the enhancement by TFA can be significant in cold and polluted areas, which provides the perspective of the realistic role of TFA in different atmospheric environments.
Arshad Arjunan Nair and Fangqun Yu
Atmos. Chem. Phys., 20, 12853–12869, https://doi.org/10.5194/acp-20-12853-2020, https://doi.org/10.5194/acp-20-12853-2020, 2020
Short summary
Short summary
Small particles in the atmosphere can affect cloud formation and properties and thus Earth's energy budget. These cloud condensation nuclei (CCN) contribute the largest uncertainties in climate change modeling. To reduce these uncertainties, it is important to quantify CCN numbers accurately, measurements of which are sparse. We propose and evaluate a machine learning method to estimate CCN, in the absence of their direct measurements, using more common measurements of weather and air quality.
Katherine R. Travis, Colette L. Heald, Hannah M. Allen, Eric C. Apel, Stephen R. Arnold, Donald R. Blake, William H. Brune, Xin Chen, Róisín Commane, John D. Crounse, Bruce C. Daube, Glenn S. Diskin, James W. Elkins, Mathew J. Evans, Samuel R. Hall, Eric J. Hintsa, Rebecca S. Hornbrook, Prasad S. Kasibhatla, Michelle J. Kim, Gan Luo, Kathryn McKain, Dylan B. Millet, Fred L. Moore, Jeffrey Peischl, Thomas B. Ryerson, Tomás Sherwen, Alexander B. Thames, Kirk Ullmann, Xuan Wang, Paul O. Wennberg, Glenn M. Wolfe, and Fangqun Yu
Atmos. Chem. Phys., 20, 7753–7781, https://doi.org/10.5194/acp-20-7753-2020, https://doi.org/10.5194/acp-20-7753-2020, 2020
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Atmospheric models overestimate the rate of removal of trace gases by the hydroxyl radical (OH). This is a concern for studies of the climate and air quality impacts of human activities. Here, we evaluate the performance of a commonly used model of atmospheric chemistry against data from the NASA Atmospheric Tomography Mission (ATom) over the remote oceans where models have received little validation. The model is generally successful, suggesting that biases in OH may be a concern over land.
Gan Luo, Fangqun Yu, and Jonathan M. Moch
Geosci. Model Dev., 13, 2879–2903, https://doi.org/10.5194/gmd-13-2879-2020, https://doi.org/10.5194/gmd-13-2879-2020, 2020
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This work improved pH calculation for cloud, rain, and wet surfaces, fraction of cloud available for aqueous-phase chemistry, rainout efficiencies for various types of cloud, empirical washout by rain and snow, and wet surface uptake in GEOS-Chem v12.6.0. We compared simulated mass concentrations of aerosol precursors and aerosols with surface monitoring networks, Arctic sites, and ATom observations, and showed that the model results with the updated wet processes agree better for most species.
Fangqun Yu, Alexey B. Nadykto, Gan Luo, and Jason Herb
Geosci. Model Dev., 13, 2663–2670, https://doi.org/10.5194/gmd-13-2663-2020, https://doi.org/10.5194/gmd-13-2663-2020, 2020
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Secondary particles formed via nucleation have important implications for air quality and climate. Here we describe nucleation rate lookup tables for four different nucleation mechanisms that can be readily used in chemistry transport and climate models. The nucleation rates predicted have been assessed against state-of-the-art laboratory measurements. The lookup tables cover a wide range of key parameters controlling binary, ternary, and ion-mediated nucleation in the Earth's atmosphere.
Fangqun Yu, Gan Luo, Arshad Arjunan Nair, James J. Schwab, James P. Sherman, and Yanda Zhang
Atmos. Chem. Phys., 20, 2591–2601, https://doi.org/10.5194/acp-20-2591-2020, https://doi.org/10.5194/acp-20-2591-2020, 2020
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Particle number concentration (PNC) is a key parameter important for the health and climate impacts of atmospheric aerosols. We show that, even during wintertime, regional nucleation occurs and contributes significantly to number concentrations of ultrafine particles and cloud condensation nuclei. Due to low biogenic emissions, wintertime regional nucleation is solely controlled by inorganic species, and ternary ion-mediated nucleation is able to capture the observed variations in PNC.
Xiaoyan Ma, Hailing Jia, Rong Tian, Fangqun Yu, and Jiagnan Li
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-54, https://doi.org/10.5194/acp-2020-54, 2020
Preprint withdrawn
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BC Mixing state, is one of critical microphysical properties to modulate optical properties, radiative forcing (RF), and climatic effect. However, it has been simply assumed previously as either external or internal mixing. In this study, by employing a nested GEOS-Chem-APM with predicted BC mixing state, we examined the effect of mixing state on aerosol optical properties, RF, and heating rate over East Asia. This will improve the predictions of aerosol climatic effect in the future.
Gan Luo, Fangqun Yu, and James Schwab
Geosci. Model Dev., 12, 3439–3447, https://doi.org/10.5194/gmd-12-3439-2019, https://doi.org/10.5194/gmd-12-3439-2019, 2019
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GEOS-Chem 12.0.0 has been recognized to significantly overestimate the concentrations of gaseous nitric acid, aerosol nitrate, and aerosol ammonium over the United States. In this study, we show that most or all of the overestimation issue appears to be associated with wet scavenging processes. With the updated wet scavenging scheme in this work, we successfully improve the skill of the model in predicting the three species concentrations, which are important for air quality and climate studies.
George S. Fanourgakis, Maria Kanakidou, Athanasios Nenes, Susanne E. Bauer, Tommi Bergman, Ken S. Carslaw, Alf Grini, Douglas S. Hamilton, Jill S. Johnson, Vlassis A. Karydis, Alf Kirkevåg, John K. Kodros, Ulrike Lohmann, Gan Luo, Risto Makkonen, Hitoshi Matsui, David Neubauer, Jeffrey R. Pierce, Julia Schmale, Philip Stier, Kostas Tsigaridis, Twan van Noije, Hailong Wang, Duncan Watson-Parris, Daniel M. Westervelt, Yang Yang, Masaru Yoshioka, Nikos Daskalakis, Stefano Decesari, Martin Gysel-Beer, Nikos Kalivitis, Xiaohong Liu, Natalie M. Mahowald, Stelios Myriokefalitakis, Roland Schrödner, Maria Sfakianaki, Alexandra P. Tsimpidi, Mingxuan Wu, and Fangqun Yu
Atmos. Chem. Phys., 19, 8591–8617, https://doi.org/10.5194/acp-19-8591-2019, https://doi.org/10.5194/acp-19-8591-2019, 2019
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Effects of aerosols on clouds are important for climate studies but are among the largest uncertainties in climate projections. This study evaluates the skill of global models to simulate aerosol, cloud condensation nuclei (CCN) and cloud droplet number concentrations (CDNCs). Model results show reduced spread in CDNC compared to CCN due to the negative correlation between the sensitivities of CDNC to aerosol number concentration (air pollution) and updraft velocity (atmospheric dynamics).
Fangqun Yu, Alexey B. Nadykto, Jason Herb, Gan Luo, Kirill M. Nazarenko, and Lyudmila A. Uvarova
Atmos. Chem. Phys., 18, 17451–17474, https://doi.org/10.5194/acp-18-17451-2018, https://doi.org/10.5194/acp-18-17451-2018, 2018
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Aerosol nucleation exerts important influences on the climate, hydrological cycle, and air quality. We have developed an advanced physical–chemical model that describes ion-induced and neutral nucleation involving ammonia, sulfuric acid, and water vapors. The model is shown to reproduce laboratory measurements taken under a wide range of conditions, offers physiochemical insights into the ternary nucleation process, and provides an accurate approach to calculate ternary rate in the atmosphere.
Jingbo Mao, Fangqun Yu, Yan Zhang, Jingyu An, Lin Wang, Jun Zheng, Lei Yao, Gan Luo, Weichun Ma, Qi Yu, Cheng Huang, Li Li, and Limin Chen
Atmos. Chem. Phys., 18, 7933–7950, https://doi.org/10.5194/acp-18-7933-2018, https://doi.org/10.5194/acp-18-7933-2018, 2018
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A few pptv of gaseous amines have been observed to affect particle nucleation and growth, and it is necessary to understand the sources and concentrations of atmospheric amines. This study presents the source-dependent amines to ammonia emission ratios and simulates methylamines concentrations in a polluted region in China with WRF-Chem. The performance of simulations based on source-dependent ratios is much better than those based on fixed ratios that have been assumed in all previous studies.
Maria Sand, Bjørn H. Samset, Yves Balkanski, Susanne Bauer, Nicolas Bellouin, Terje K. Berntsen, Huisheng Bian, Mian Chin, Thomas Diehl, Richard Easter, Steven J. Ghan, Trond Iversen, Alf Kirkevåg, Jean-François Lamarque, Guangxing Lin, Xiaohong Liu, Gan Luo, Gunnar Myhre, Twan van Noije, Joyce E. Penner, Michael Schulz, Øyvind Seland, Ragnhild B. Skeie, Philip Stier, Toshihiko Takemura, Kostas Tsigaridis, Fangqun Yu, Kai Zhang, and Hua Zhang
Atmos. Chem. Phys., 17, 12197–12218, https://doi.org/10.5194/acp-17-12197-2017, https://doi.org/10.5194/acp-17-12197-2017, 2017
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The role of aerosols in the changing polar climate is not well understood and the aerosols are poorly constrained in the models. In this study we have compared output from 16 different aerosol models with available observations at both poles. We show that the model median is representative of the observations, but the model spread is large. The Arctic direct aerosol radiative effect over the industrial area is positive during spring due to black carbon and negative during summer due to sulfate.
Fangqun Yu, Gan Luo, Alexey B. Nadykto, and Jason Herb
Atmos. Chem. Phys., 17, 4997–5005, https://doi.org/10.5194/acp-17-4997-2017, https://doi.org/10.5194/acp-17-4997-2017, 2017
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H2SO4–organics clustering thermodynamics from quantum studies has been employed to develop a scheme to include temperature dependence in an H2SO4–organics nucleation parameterization. We show that temperature has a strong impact on nucleation rates, particle number concentrations, and aerosol first indirect radiative forcing in summer. To our knowledge, the study represents the first attempt to study the temperature effect on organics-mediated nucleation in the global atmosphere.
F. Yu, G. Luo, S. C. Pryor, P. R. Pillai, S. H. Lee, J. Ortega, J. J. Schwab, A. G. Hallar, W. R. Leaitch, V. P. Aneja, J. N. Smith, J. T. Walker, O. Hogrefe, and K. L. Demerjian
Atmos. Chem. Phys., 15, 13993–14003, https://doi.org/10.5194/acp-15-13993-2015, https://doi.org/10.5194/acp-15-13993-2015, 2015
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The role of low-volatility organics in new particle formation (NPF) in the atmosphere is assessed. An empirical formulation in which formation rate is a function of the concentrations of sulfuric acid and low-volatility organics significantly overpredicts NPF in the summer.
Two different schemes predict quite different nucleation rates (including their spatial patterns), concentrations of cloud condensation nuclei, and aerosol first indirect radiative forcing in North America.
G. W. Mann, K. S. Carslaw, C. L. Reddington, K. J. Pringle, M. Schulz, A. Asmi, D. V. Spracklen, D. A. Ridley, M. T. Woodhouse, L. A. Lee, K. Zhang, S. J. Ghan, R. C. Easter, X. Liu, P. Stier, Y. H. Lee, P. J. Adams, H. Tost, J. Lelieveld, S. E. Bauer, K. Tsigaridis, T. P. C. van Noije, A. Strunk, E. Vignati, N. Bellouin, M. Dalvi, C. E. Johnson, T. Bergman, H. Kokkola, K. von Salzen, F. Yu, G. Luo, A. Petzold, J. Heintzenberg, A. Clarke, J. A. Ogren, J. Gras, U. Baltensperger, U. Kaminski, S. G. Jennings, C. D. O'Dowd, R. M. Harrison, D. C. S. Beddows, M. Kulmala, Y. Viisanen, V. Ulevicius, N. Mihalopoulos, V. Zdimal, M. Fiebig, H.-C. Hansson, E. Swietlicki, and J. S. Henzing
Atmos. Chem. Phys., 14, 4679–4713, https://doi.org/10.5194/acp-14-4679-2014, https://doi.org/10.5194/acp-14-4679-2014, 2014
X. Ma, K. Bartlett, K. Harmon, and F. Yu
Atmos. Meas. Tech., 6, 2391–2401, https://doi.org/10.5194/amt-6-2391-2013, https://doi.org/10.5194/amt-6-2391-2013, 2013
Related subject area
Subject: Aerosols | Research Activity: Atmospheric Modelling | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Simulating the radiative forcing of oceanic dimethylsulfide (DMS) in Asia based on machine learning estimates
Quantifying the effects of mixing state on aerosol optical properties
Secondary organic aerosol formation via multiphase reaction of hydrocarbons in urban atmospheres using CAMx integrated with the UNIPAR model
Contrasting source contributions of Arctic black carbon to atmospheric concentrations, deposition flux, and atmospheric and snow radiative effects
Effect of dust on rainfall over the Red Sea coast based on WRF-Chem model simulations
A new assessment of global and regional budgets, fluxes, and lifetimes of atmospheric reactive N and S gases and aerosols
Limitations in representation of physical processes prevent successful simulation of PM2.5 during KORUS-AQ
Eurodelta multi-model simulated and observed particulate matter trends in Europe in the period of 1990–2010
Elucidating the critical oligomeric steps in secondary organic aerosol and brown carbon formation
Fast climate responses to emission reductions in aerosol and ozone precursors in China during 2013–2017
Secondary PM2.5 decreases significantly less than NO2 emission reductions during COVID lockdown in Germany
Molecular-level nucleation mechanism of iodic acid and methanesulfonic acid
Estimation of secondary PM2.5 in China and the United States using a multi-tracer approach
Two-way coupled meteorology and air quality models in Asia: a systematic review and meta-analysis of impacts of aerosol feedbacks on meteorology and air quality
OCEANFILMS (Organic Compounds from Ecosystems to Aerosols: Natural Films and Interfaces via Langmuir Molecular Surfactants) sea spray organic aerosol emissions – implementation in a global climate model and impacts on clouds
The pathway of impacts of aerosol direct effects on secondary inorganic aerosol formation
The impact of molecular self-organisation on the atmospheric fate of a cooking aerosol proxy
The formation and mitigation of nitrate pollution: comparison between urban and suburban environments
Statistical and machine learning methods for evaluating trends in air quality under changing meteorological conditions
Impacts of aerosol–photolysis interaction and aerosol–radiation feedback on surface-layer ozone in North China during multi-pollutant air pollution episodes
Reducing future air-pollution-related premature mortality over Europe by mitigating emissions from the energy sector: assessing an 80 % renewable energies scenario
The impact of chlorine chemistry combined with heterogeneous N2O5 reactions on air quality in China
OH-initiated atmospheric degradation of hydroxyalkyl hydroperoxides: mechanism, kinetics, and structure–activity relationship
A predictive viscosity model for aqueous electrolytes and mixed organic–inorganic aerosol phases
Impact of urban heat island on inorganic aerosol in the lower free troposphere: a case study in Hangzhou, China
The role of organic acids in new particle formation from methanesulfonic acid and methylamine
The number fraction of iron-containing particles affects OH, HO2 and H2O2 budgets in the atmospheric aqueous phase
Source-resolved variability of fine particulate matter and human exposure in an urban area
The impact of atmospheric blocking on the compounding effect of ozone pollution and temperature: a copula-based approach
Exploring dimethyl sulfide (DMS) oxidation and implications for global aerosol radiative forcing
Modelling changes in secondary inorganic aerosol formation and nitrogen deposition in Europe from 2005 to 2030
Extension of the AIOMFAC model by iodine and carbonate species: applications for aerosol acidity and cloud droplet activation
A numerical framework for simulating the atmospheric variability of supermicron marine biogenic ice nucleating particles
Prediction of secondary organic aerosol from the multiphase reaction of gasoline vapor by using volatility–reactivity base lumping
Modelling the gas–particle partitioning and water uptake of isoprene-derived secondary organic aerosol at high and low relative humidity
Evaluation of WRF-CHIMERE coupled models for the simulation of PM2.5 in large East African urban conurbations
Modeling secondary organic aerosol formation from volatile chemical products
Why is the city's responsibility for its air pollution often underestimated? A focus on PM2.5
Impact of reduced emissions on direct and indirect aerosol radiative forcing during COVID–19 lockdown in Europe
Quantifying the structural uncertainty of the aerosol mixing state representation in a modal model
Changes in PM2.5 concentrations and their sources in the US from 1990 to 2010
A predictive thermodynamic framework of cloud droplet activation for chemically unresolved aerosol mixtures, including surface tension, non-ideality, and bulk–surface partitioning
Process-based and observation-constrained SOA simulations in China: the role of semivolatile and intermediate-volatility organic compounds and OH levels
Impacts of emission changes in China from 2010 to 2017 on domestic and intercontinental air quality and health effect
Exploring the sensitivity of atmospheric nitrate concentrations to nitric acid uptake rate using the Met Office's Unified Model
Improving the representation of HONO chemistry in CMAQ and examining its impact on haze over China
How alkaline compounds control atmospheric aerosol particle acidity
Aerosol transport pathways and source attribution in China during the COVID-19 outbreak
Nonlinear responses of particulate nitrate to NOx emission controls in the megalopolises of China
Insight into PM2.5 sources by applying positive matrix factorization (PMF) at urban and rural sites of Beijing
Junri Zhao, Weichun Ma, Kelsey R. Bilsback, Jeffrey R. Pierce, Shengqian Zhou, Ying Chen, Guipeng Yang, and Yan Zhang
Atmos. Chem. Phys., 22, 9583–9600, https://doi.org/10.5194/acp-22-9583-2022, https://doi.org/10.5194/acp-22-9583-2022, 2022
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Marine dimethylsulfide (DMS) emissions play important roles in atmospheric sulfur cycle and climate effects. In this study, DMS emissions were estimated by using the machine learning method and drove the global 3D chemical transport model to simulate their climate effects. To our knowledge, this is the first study in the Asian region that quantifies the combined impacts of DMS on sulfate, particle number concentration, and radiative forcings.
Yu Yao, Jeffrey H. Curtis, Joseph Ching, Zhonghua Zheng, and Nicole Riemer
Atmos. Chem. Phys., 22, 9265–9282, https://doi.org/10.5194/acp-22-9265-2022, https://doi.org/10.5194/acp-22-9265-2022, 2022
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Investigating the impacts of aerosol mixing state on aerosol optical properties has a long history from both the modeling and experimental perspective. In this study, we used particle-resolved simulations as a benchmark to determine the error in optical properties when using simplified aerosol representations. We found that errors in single scattering albedo due to the internal mixture assumptions can have substantial effects on calculating aerosol direct radiative forcing.
Zechen Yu, Myoseon Jang, Soontae Kim, Kyuwon Son, Sanghee Han, Azad Madhu, and Jinsoo Park
Atmos. Chem. Phys., 22, 9083–9098, https://doi.org/10.5194/acp-22-9083-2022, https://doi.org/10.5194/acp-22-9083-2022, 2022
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The UNIPAR model was incorporated into CAMx to predict the ambient concentration of organic matter in urban atmospheres during the KORUS-AQ campaign. CAMx–UNIPAR significantly improved the simulation of SOA formation under the wet aerosol condition through the consideration of aqueous reactions of reactive organic species and gas–aqueous partitioning into the wet inorganic aerosol.
Hitoshi Matsui, Tatsuhiro Mori, Sho Ohata, Nobuhiro Moteki, Naga Oshima, Kumiko Goto-Azuma, Makoto Koike, and Yutaka Kondo
Atmos. Chem. Phys., 22, 8989–9009, https://doi.org/10.5194/acp-22-8989-2022, https://doi.org/10.5194/acp-22-8989-2022, 2022
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Using a global aerosol model, we find that the source contributions to radiative effects of black carbon (BC) in the Arctic are quite different from those to mass concentrations and deposition flux of BC in the Arctic. This is because microphysical properties (e.g., mixing state), altitudes, and seasonal variations of BC in the atmosphere differ among emissions sources. These differences need to be considered for accurate simulations of Arctic BC and its source contributions and climate impacts.
Sagar P. Parajuli, Georgiy L. Stenchikov, Alexander Ukhov, Suleiman Mostamandi, Paul A. Kucera, Duncan Axisa, William I. Gustafson Jr., and Yannian Zhu
Atmos. Chem. Phys., 22, 8659–8682, https://doi.org/10.5194/acp-22-8659-2022, https://doi.org/10.5194/acp-22-8659-2022, 2022
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Rainfall affects the distribution of surface- and groundwater resources, which are constantly declining over the Middle East and North Africa (MENA) due to overexploitation. Here, we explored the effects of dust on rainfall using WRF-Chem model simulations. Although dust is considered a nuisance from an air quality perspective, our results highlight the positive fundamental role of dust particles in modulating rainfall formation and distribution, which has implications for cloud seeding.
Yao Ge, Massimo Vieno, David S. Stevenson, Peter Wind, and Mathew R. Heal
Atmos. Chem. Phys., 22, 8343–8368, https://doi.org/10.5194/acp-22-8343-2022, https://doi.org/10.5194/acp-22-8343-2022, 2022
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Reactive N and S gases and aerosols are critical determinants of air quality. We report a comprehensive analysis of the concentrations, wet and dry deposition, fluxes, and lifetimes of these species globally as well as for 10 world regions. We used the EMEP MSC-W model coupled with WRF meteorology and 2015 global emissions. Our work demonstrates the substantial regional variation in these quantities and the need for modelling to simulate atmospheric responses to precursor emissions.
Katherine R. Travis, James H. Crawford, Gao Chen, Carolyn E. Jordan, Benjamin A. Nault, Hwajin Kim, Jose L. Jimenez, Pedro Campuzano-Jost, Jack E. Dibb, Jung-Hun Woo, Younha Kim, Shixian Zhai, Xuan Wang, Erin E. McDuffie, Gan Luo, Fangqun Yu, Saewung Kim, Isobel J. Simpson, Donald R. Blake, Limseok Chang, and Michelle J. Kim
Atmos. Chem. Phys., 22, 7933–7958, https://doi.org/10.5194/acp-22-7933-2022, https://doi.org/10.5194/acp-22-7933-2022, 2022
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The 2016 Korea–United States Air Quality (KORUS-AQ) field campaign provided a unique set of observations to improve our understanding of PM2.5 pollution in South Korea. Models typically have errors in simulating PM2.5 in this region, which is of concern for the development of control measures. We use KORUS-AQ observations to improve our understanding of the mechanisms driving PM2.5 and the implications of model errors for determining PM2.5 that is attributable to local or foreign sources.
Svetlana Tsyro, Wenche Aas, Augustin Colette, Camilla Andersson, Bertrand Bessagnet, Giancarlo Ciarelli, Florian Couvidat, Kees Cuvelier, Astrid Manders, Kathleen Mar, Mihaela Mircea, Noelia Otero, Maria-Teresa Pay, Valentin Raffort, Yelva Roustan, Mark R. Theobald, Marta G. Vivanco, Hilde Fagerli, Peter Wind, Gino Briganti, Andrea Cappelletti, Massimo D'Isidoro, and Mario Adani
Atmos. Chem. Phys., 22, 7207–7257, https://doi.org/10.5194/acp-22-7207-2022, https://doi.org/10.5194/acp-22-7207-2022, 2022
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Particulate matter (PM) air pollution causes adverse health effects. In Europe, the emissions caused by anthropogenic activities have been reduced in the last decades. To assess the efficiency of emission reductions in improving air quality, we have studied the evolution of PM pollution in Europe. Simulations with six air quality models and observational data indicate a decrease in PM concentrations by 10 % to 30 % across Europe from 2000 to 2010, which is mainly a result of emission reductions.
Yuemeng Ji, Qiuju Shi, Xiaohui Ma, Lei Gao, Jiaxin Wang, Yixin Li, Yanpeng Gao, Guiying Li, Renyi Zhang, and Taicheng An
Atmos. Chem. Phys., 22, 7259–7271, https://doi.org/10.5194/acp-22-7259-2022, https://doi.org/10.5194/acp-22-7259-2022, 2022
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The formation mechanisms of secondary organic aerosol and brown carbon from small α-carbonyls are still unclear. Thus, the mechanisms and kinetics of aqueous-phase reactions of glyoxal were investigated using quantum chemical and kinetic rate calculations. Several essential isomeric processes were identified, including protonation to yield diol/tetrol and carbenium ions as well as nucleophilic addition of carbenium ions to diol/tetrol and free methylamine/ammonia.
Jiyuan Gao, Yang Yang, Hailong Wang, Pinya Wang, Huimin Li, Mengyun Li, Lili Ren, Xu Yue, and Hong Liao
Atmos. Chem. Phys., 22, 7131–7142, https://doi.org/10.5194/acp-22-7131-2022, https://doi.org/10.5194/acp-22-7131-2022, 2022
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China has been implementing a sequence of policies for clean air since the year 2013. The aerosol decline produced a 0.09 ± 0.10°C warming during 2013–2017 estimated in this study, and the increase in ozone in the lower troposphere during this time period accelerated the warming, leading to a total 0.16 ± 0.15°C temperature increase in eastern China. Residential emission reductions led to a cooling effect because of a substantial decrease in light-absorbing aerosols.
Vigneshkumar Balamurugan, Jia Chen, Zhen Qu, Xiao Bi, and Frank N. Keutsch
Atmos. Chem. Phys., 22, 7105–7129, https://doi.org/10.5194/acp-22-7105-2022, https://doi.org/10.5194/acp-22-7105-2022, 2022
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In this study, we investigated the response of secondary pollutants to changes in precursor emissions, focusing on the formation of secondary PM, during the COVID-19 lockdown period. We show that, due to the decrease in primary NOx emissions, atmospheric oxidizing capacity is increased. The nighttime increase in ozone, caused by less NO titration, results in higher NO3 radicals, which contribute significantly to the formation of PM nitrates. O3 should be limited in order to control PM pollution.
An Ning, Ling Liu, Lin Ji, and Xiuhui Zhang
Atmos. Chem. Phys., 22, 6103–6114, https://doi.org/10.5194/acp-22-6103-2022, https://doi.org/10.5194/acp-22-6103-2022, 2022
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Iodic acid (IA) and methanesulfonic acid (MSA) were previously proved to be significant nucleation precursors in marine areas. However, the nucleation process involved in IA and MSA remains unclear. We show the enhancement of MSA on IA cluster formation and reveal the IAM-SA nucleating mechanism using a theoretical approach. This study helps to understand the clustering process in which marine sulfur- and iodine-containing species are jointly involved and its impact on new particle formation.
Haoran Zhang, Nan Li, Keqin Tang, Hong Liao, Chong Shi, Cheng Huang, Hongli Wang, Song Guo, Min Hu, Xinlei Ge, Mindong Chen, Zhenxin Liu, Huan Yu, and Jianlin Hu
Atmos. Chem. Phys., 22, 5495–5514, https://doi.org/10.5194/acp-22-5495-2022, https://doi.org/10.5194/acp-22-5495-2022, 2022
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We developed a new algorithm with low economic/technique costs to identify primary and secondary components of PM2.5. Our model was shown to be reliable by comparison with different observation datasets. We systematically explored the patterns and changes in the secondary PM2.5 pollution in China at large spatial and time scales. We believe that this method is a promising tool for efficiently estimating primary and secondary PM2.5, and has huge potential for future PM mitigation.
Chao Gao, Aijun Xiu, Xuelei Zhang, Qingqing Tong, Hongmei Zhao, Shichun Zhang, Guangyi Yang, and Mengduo Zhang
Atmos. Chem. Phys., 22, 5265–5329, https://doi.org/10.5194/acp-22-5265-2022, https://doi.org/10.5194/acp-22-5265-2022, 2022
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With ever-growing applications of two-way coupled meteorology and air quality models in Asia over the past decade, this paper summarizes the current status and research focuses, as well as how aerosol effects impact model performance, meteorology, and air quality. These models enable investigations of ARI and ACI effects induced by natural and anthropogenic aerosols in Asia, which has serious air pollution problems. The current gaps and perspectives are also presented and discussed.
Susannah M. Burrows, Richard C. Easter, Xiaohong Liu, Po-Lun Ma, Hailong Wang, Scott M. Elliott, Balwinder Singh, Kai Zhang, and Philip J. Rasch
Atmos. Chem. Phys., 22, 5223–5251, https://doi.org/10.5194/acp-22-5223-2022, https://doi.org/10.5194/acp-22-5223-2022, 2022
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Sea spray particles are composed of a mixture of salts and organic substances from oceanic microorganisms. In prior work, our team developed an approach connecting sea spray chemistry to ocean biology, called OCEANFILMS. Here we describe its implementation within an Earth system model, E3SM. We show that simulated sea spray chemistry is consistent with observed seasonal cycles and that sunlight reflected by simulated Southern Ocean clouds increases, consistent with analysis of satellite data.
Jiandong Wang, Jia Xing, Shuxiao Wang, Rohit Mathur, Jiaping Wang, Yuqiang Zhang, Chao Liu, Jonathan Pleim, Dian Ding, Xing Chang, Jingkun Jiang, Peng Zhao, Shovan Kumar Sahu, Yuzhi Jin, David C. Wong, and Jiming Hao
Atmos. Chem. Phys., 22, 5147–5156, https://doi.org/10.5194/acp-22-5147-2022, https://doi.org/10.5194/acp-22-5147-2022, 2022
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Aerosols reduce surface solar radiation and change the photolysis rate and planetary boundary layer stability. In this study, the online coupled meteorological and chemistry model was used to explore the detailed pathway of how aerosol direct effects affect secondary inorganic aerosol. The effects through the dynamics pathway act as an equally or even more important route compared with the photolysis pathway in affecting secondary aerosol concentration in both summer and winter.
Adam Milsom, Adam M. Squires, Andrew D. Ward, and Christian Pfrang
Atmos. Chem. Phys., 22, 4895–4907, https://doi.org/10.5194/acp-22-4895-2022, https://doi.org/10.5194/acp-22-4895-2022, 2022
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Cooking emissions can self-organise into nanostructured lamellar bilayers, and this can influence reaction kinetics. We developed a kinetic multi-layer model-based description of decay data we obtained from laboratory experiments of the ozonolysis of coated films of such a self-organised system, demonstrating a decreased diffusivity for both oleic acid and ozone. Nanostructure formation can thus increase the reactive half-life of oleic acid by days under typical indoor and outdoor conditions.
Suxia Yang, Bin Yuan, Yuwen Peng, Shan Huang, Wei Chen, Weiwei Hu, Chenglei Pei, Jun Zhou, David D. Parrish, Wenjie Wang, Xianjun He, Chunlei Cheng, Xiao-Bing Li, Xiaoyun Yang, Yu Song, Haichao Wang, Jipeng Qi, Baolin Wang, Chen Wang, Chaomin Wang, Zelong Wang, Tiange Li, E Zheng, Sihang Wang, Caihong Wu, Mingfu Cai, Chenshuo Ye, Wei Song, Peng Cheng, Duohong Chen, Xinming Wang, Zhanyi Zhang, Xuemei Wang, Junyu Zheng, and Min Shao
Atmos. Chem. Phys., 22, 4539–4556, https://doi.org/10.5194/acp-22-4539-2022, https://doi.org/10.5194/acp-22-4539-2022, 2022
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We use a model constrained using observations to study the formation of nitrate aerosol in and downwind of a representative megacity. We found different contributions of various chemical reactions to ground-level nitrate concentrations between urban and suburban regions. We also show that controlling VOC emissions are effective for decreasing nitrate formation in both urban and regional environments, although VOCs are not direct precursors of nitrate aerosol.
Minghao Qiu, Corwin M. Zigler, and Noelle E. Selin
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-232, https://doi.org/10.5194/acp-2022-232, 2022
Revised manuscript accepted for ACP
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Evaluating impacts of emission changes on air quality requires accounting for meteorological variability. Many studies use simple regression methods to correct for meteorology, but much less is known about their performance. Using cases in US and China, we show that widely-used regression models do not perform well and can lead to biased estimates of emission-driven trends. We propose a novel machine learning method with lower bias and provide recommendations to policy makers and researchers.
Hao Yang, Lei Chen, Hong Liao, Jia Zhu, Wenjie Wang, and Xin Li
Atmos. Chem. Phys., 22, 4101–4116, https://doi.org/10.5194/acp-22-4101-2022, https://doi.org/10.5194/acp-22-4101-2022, 2022
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Aerosols can influence O3 through aerosol–radiation interactions, including aerosol–photolysis interaction (API) and aerosol–radiation feedback (ARF). The weakened photolysis rates and changed meteorological conditions reduce surface-layer O3 concentrations by up to 9.3–11.4 ppb, with API and ARF contributing 74.6 %–90.0 % and 10.0 %–25.4 % of the O3 decrease in three episodes, respectively, which indicates that API is the dominant way for O3 reduction related to aerosol–radiation interactions.
Patricia Tarín-Carrasco, Ulas Im, Camilla Geels, Laura Palacios-Peña, and Pedro Jiménez-Guerrero
Atmos. Chem. Phys., 22, 3945–3965, https://doi.org/10.5194/acp-22-3945-2022, https://doi.org/10.5194/acp-22-3945-2022, 2022
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The evidence of the effects of atmospheric pollution (and particularly fine particulate matter, PM2.5) on human mortality is now unquestionable. Here, 895 000 annual premature deaths (PD) are estimated for the present (1991–2010), which increases to 1 540 000 in the year 2050 due to the ageing of the European population. The implementation of a mitigation scenario (80 % of the energy production in Europe from renewable sources) could lead to a decrease of over 60 000 annual PD for the year 2050.
Xiajie Yang, Qiaoqiao Wang, Nan Ma, Weiwei Hu, Yang Gao, Zhijiong Huang, Junyu Zheng, Bin Yuan, Ning Yang, Jiangchuan Tao, Juan Hong, Yafang Cheng, and Hang Su
Atmos. Chem. Phys., 22, 3743–3762, https://doi.org/10.5194/acp-22-3743-2022, https://doi.org/10.5194/acp-22-3743-2022, 2022
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We use the GEOS-Chem model with additional anthropogenic and biomass burning chlorine emissions combined with updated parameterizations for N2O5 ＋ Cl chemistry to investigate the impacts of chlorine chemistry on air quality in China. Our study not only significantly improves the model's performance but also demonstrates the importance of non-sea-salt chlorine sources as well as an appropriate parameterization for N2O5 ＋ Cl chemistry to the impact of chlorine chemistry in China.
Long Chen, Yu Huang, Yonggang Xue, Zhihui Jia, and Wenliang Wang
Atmos. Chem. Phys., 22, 3693–3711, https://doi.org/10.5194/acp-22-3693-2022, https://doi.org/10.5194/acp-22-3693-2022, 2022
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Quantum chemical methods are applied to gain insight into the detailed mechanisms of OH-initiated oxidation of distinct HHPs. The dominant pathway is H-abstraction from the -OOH group in the initiation reactions of the OH radical with HOCH2OOH and HOC(CH3)2OOH. H-abstraction from -CH group is competitive with that from the -OOH group in the reaction of the OH radical with HOCH(CH3)OOH. The barrier of H-abstraction from the -OOH group is slightly increased as the methyl group number increases.
Joseph Lilek and Andreas Zuend
Atmos. Chem. Phys., 22, 3203–3233, https://doi.org/10.5194/acp-22-3203-2022, https://doi.org/10.5194/acp-22-3203-2022, 2022
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Depending on temperature and chemical makeup, certain aerosols can be highly viscous or glassy, with atmospheric implications. We have therefore implemented two major upgrades to the predictive viscosity model AIOMFAC-VISC. First, we created a new viscosity model for aqueous electrolyte solutions containing an arbitrary number of ion species. Second, we integrated the electrolyte model within the existing AIOMFAC-VISC framework to enable viscosity predictions for organic–inorganic mixtures.
Hanqing Kang, Bin Zhu, Gerrit de Leeuw, Bu Yu, Ronald J. van der A, and Wen Lu
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-93, https://doi.org/10.5194/acp-2022-93, 2022
Revised manuscript accepted for ACP
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This study quantified the contribution of each urban-induced meteorological effect (temperature, humidity, and circulation) to aerosol concentration. We found that the urban heat island (UHI) circulation dominates the UHI effects on aerosol. The UHI circulation transports aerosol and its precursor gases from warmer lower boundary layer to colder lower free troposphere and promotes the secondary formation of ammonium nitrate aerosol in the cold atmosphere.
Rongjie Zhang, Jiewen Shen, Hong-Bin Xie, Jingwen Chen, and Jonas Elm
Atmos. Chem. Phys., 22, 2639–2650, https://doi.org/10.5194/acp-22-2639-2022, https://doi.org/10.5194/acp-22-2639-2022, 2022
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Formic acid is screened out as the species that can effectively catalyze the new particle formation (NPF) of the methanesulfonic acid (MSA)–methylamine system, indicating organic acids might be required to facilitate MSA-driven NPF in the atmosphere. The results are significant to comprehensively understand the MSA-driven NPF and expand current knowledge of the contribution of OAs to NPF.
Amina Khaled, Minghui Zhang, and Barbara Ervens
Atmos. Chem. Phys., 22, 1989–2009, https://doi.org/10.5194/acp-22-1989-2022, https://doi.org/10.5194/acp-22-1989-2022, 2022
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Chemical reactions with iron in clouds and aerosol form and cycle reactive oxygen species (ROS). Previous model studies assumed that all cloud droplets (particles) contain iron, while single-particle analyses showed otherwise. By means of a model, we explore the bias in predicted ROS budgets by distributing a given iron mass to either all or only a few droplets (particles). Implications for oxidation potential, radical loss and iron oxidation state are discussed.
Pablo Garcia Rivera, Brian T. Dinkelacker, Ioannis Kioutsioukis, Peter J. Adams, and Spyros N. Pandis
Atmos. Chem. Phys., 22, 2011–2027, https://doi.org/10.5194/acp-22-2011-2022, https://doi.org/10.5194/acp-22-2011-2022, 2022
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The contribution of various pollution sources to the variability of fine PM in an urban area was examined using as an example the city of Pittsburgh. Biomass burning aerosol shows the largest variability during the winter with local maxima within the city and in the suburbs. During both periods the largest contributing source to the average PM2.5 is particles from outside the modeling domain. The average population-weighted PM2.5 concentration does not change significantly with resolution.
Noelia Otero, Oscar E. Jurado, Tim Butler, and Henning W. Rust
Atmos. Chem. Phys., 22, 1905–1919, https://doi.org/10.5194/acp-22-1905-2022, https://doi.org/10.5194/acp-22-1905-2022, 2022
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Surface ozone and temperature are strongly dependent and their extremes might be exacerbated by underlying climatological drivers, such as atmospheric blocking. Using an observational data set, we measure the dependence structure between ozone and temperature under the influence of atmospheric blocking. Blocks enhanced the probability of occurrence of compound ozone and temperature extremes over northwestern and central Europe, leading to greater health risks.
Ka Ming Fung, Colette L. Heald, Jesse H. Kroll, Siyuan Wang, Duseong S. Jo, Andrew Gettelman, Zheng Lu, Xiaohong Liu, Rahul A. Zaveri, Eric C. Apel, Donald R. Blake, Jose-Luis Jimenez, Pedro Campuzano-Jost, Patrick R. Veres, Timothy S. Bates, John E. Shilling, and Maria Zawadowicz
Atmos. Chem. Phys., 22, 1549–1573, https://doi.org/10.5194/acp-22-1549-2022, https://doi.org/10.5194/acp-22-1549-2022, 2022
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Understanding the natural aerosol burden in the preindustrial era is crucial for us to assess how atmospheric aerosols affect the Earth's radiative budgets. Our study explores how a detailed description of dimethyl sulfide (DMS) oxidation (implemented in the Community Atmospheric Model version 6 with chemistry, CAM6-chem) could help us better estimate the present-day and preindustrial concentrations of sulfate and other relevant chemicals, as well as the resulting aerosol radiative impacts.
Jan Eiof Jonson, Hilde Fagerli, Thomas Scheuschner, and Svetlana Tsyro
Atmos. Chem. Phys., 22, 1311–1331, https://doi.org/10.5194/acp-22-1311-2022, https://doi.org/10.5194/acp-22-1311-2022, 2022
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Ammonia emissions are expected to decrease less than SOx and NOx emissions between 2005 and 2030. As the formation of PM2.5 particles from ammonia depends on the ratio between ammonia on one hand and sulfate (from SOx) and HNO3 (from NOx) on the other hand, the efficiency of particle formation from ammonia is decreasing. Depositions of reduced nitrogen are decreasing much less than oxidized nitrogen. The critical loads for nitrogen deposition will also be exceeded in much of Europe in 2030.
Hang Yin, Jing Dou, Liviana Klein, Ulrich K. Krieger, Alison Bain, Brandon J. Wallace, Thomas C. Preston, and Andreas Zuend
Atmos. Chem. Phys., 22, 973–1013, https://doi.org/10.5194/acp-22-973-2022, https://doi.org/10.5194/acp-22-973-2022, 2022
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Iodine and carbonate species are important components in marine and dust aerosols, respectively. We introduce an extended version of the AIOMFAC thermodynamic mixing model, which includes the ions I−, IO3−, HCO3−, CO32−, OH−, and CO2(aq) as new species, and we discuss two methods for solving the carbonate dissociation equilibria numerically. We also present new experimental water activity data for aqueous iodide and iodate systems.
Isabelle Steinke, Paul J. DeMott, Grant B. Deane, Thomas C. J. Hill, Mathew Maltrud, Aishwarya Raman, and Susannah M. Burrows
Atmos. Chem. Phys., 22, 847–859, https://doi.org/10.5194/acp-22-847-2022, https://doi.org/10.5194/acp-22-847-2022, 2022
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Over the oceans, sea spray aerosol is an important source of particles that may initiate the formation of cloud ice, which then has implications for the radiative properties of marine clouds. In our study, we focus on marine biogenic particles that are emitted episodically and develop a numerical framework to describe these emissions. We find that further cloud-resolving model studies and targeted observations are needed to fully understand the climate impacts from marine biogenic particles.
Sanghee Han and Myoseon Jang
Atmos. Chem. Phys., 22, 625–639, https://doi.org/10.5194/acp-22-625-2022, https://doi.org/10.5194/acp-22-625-2022, 2022
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The gasoline SOA formation potential was simulated by using the UNIPAR model coupled with CB6r3 mechanism under varying NOx levels, aerosol acidity, humidity, temperature, and concentrations of aqueous salts and gasoline vapor. The model predicts SOA formation via multiphase reactions in the absence of wall bias. The simulation shows that both heterogeneous reactions in the aqueous phase and the implementation of model parameters corrected for GWP are critical to accurately predict SOA mass.
Dalrin Ampritta Amaladhasan, Claudia Heyn, Christopher R. Hoyle, Imad El Haddad, Miriam Elser, Simone M. Pieber, Jay G. Slowik, Antonio Amorim, Jonathan Duplissy, Sebastian Ehrhart, Vladimir Makhmutov, Ugo Molteni, Matti Rissanen, Yuri Stozhkov, Robert Wagner, Armin Hansel, Jasper Kirkby, Neil M. Donahue, Rainer Volkamer, Urs Baltensperger, Martin Gysel-Beer, and Andreas Zuend
Atmos. Chem. Phys., 22, 215–244, https://doi.org/10.5194/acp-22-215-2022, https://doi.org/10.5194/acp-22-215-2022, 2022
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We use a combination of models for gas-phase chemical reactions and equilibrium gas–particle partitioning of isoprene-derived secondary organic aerosols (SOAs) informed by dark ozonolysis experiments conducted in the CLOUD chamber. Our predictions cover high to low relative humidities (RHs) and quantify how SOA mass yields are enhanced at high RH as well as the impact of inorganic seeds of distinct hygroscopicities and acidities on the coupled partitioning of water and semi-volatile organics.
Andrea Mazzeo, Michael Burrow, Andrew Quinn, Eloise A. Marais, Ajit Singh, David Ng'ang'a, Michael J. Gatari, and Francis D. Pope
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-552, https://doi.org/10.5194/acp-2021-552, 2022
Revised manuscript accepted for ACP
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The modelling system for meteorology and chemistry-transport processes WRF-CHIMERE has been tested and validated for three conurbations of East Africa using the most up-to-date anthropogenic emissions available. Results show that the model is able to reproduce hourly and daily temporal variability of aerosol concentrations close to observations both in urban and rural environments encouraging the adoption of numerical modelling as a tool for air quality management in East Africa.
Elyse A. Pennington, Karl M. Seltzer, Benjamin N. Murphy, Momei Qin, John H. Seinfeld, and Havala O. T. Pye
Atmos. Chem. Phys., 21, 18247–18261, https://doi.org/10.5194/acp-21-18247-2021, https://doi.org/10.5194/acp-21-18247-2021, 2021
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Volatile chemical products (VCPs) are commonly used consumer and industrial items that contribute to the formation of atmospheric aerosol. We implemented the emissions and chemistry of VCPs in a regional-scale model and compared predictions with measurements made in Los Angeles. Our results reduced model bias and suggest that VCPs may contribute up to half of anthropogenic secondary organic aerosol in Los Angeles and are an important source of human-influenced particular matter in urban areas.
Philippe Thunis, Alain Clappier, Alexander de Meij, Enrico Pisoni, Bertrand Bessagnet, and Leonor Tarrason
Atmos. Chem. Phys., 21, 18195–18212, https://doi.org/10.5194/acp-21-18195-2021, https://doi.org/10.5194/acp-21-18195-2021, 2021
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Air pollution's origin in cities is still a point of discussion, and approaches to assess the city's responsibility for its pollution are not harmonized and thus not comparable, resulting in sometimes contradicting interpretations. We show that methodological choices can easily lead to differences of a factor of 2 in terms of responsibility outcome and stress that methodological choices and assumptions most often lead to a systematic and important underestimation of the city's responsibility.
Simon Felix Reifenberg, Anna Martin, Matthias Kohl, Zaneta Hamryszczak, Ivan Tadic, Lenard Röder, Daniel J. Crowley, Horst Fischer, Katharina Kaiser, Johannes Schneider, Raphael Dörich, John N. Crowley, Laura Tomsche, Andreas Marsing, Christiane Voigt, Andreas Zahn, Christopher Pöhlker, Bruna Holanda, Ovid O. Krüger, Ulrich Pöschl, Mira Pöhlker, Patrick Jöckel, Marcel Dorf, Ulrich Schumann, Jonathan Williams, Joachim Curtius, Hardwig Harder, Hans Schlager, Jos Lelieveld, and Andrea Pozzer
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-1005, https://doi.org/10.5194/acp-2021-1005, 2021
Revised manuscript accepted for ACP
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In this work we use a combination of observational data from an aircraft campaign and model results to investigate the effect of the European lockdown due to COVID-19 in spring 2020. Using model results, we show that the largest relative changes to the atmospheric composition caused by the reduced emissionsare located in the upper troposphere, around the aircraft cruise altitude, while largest absolute changes are present at the surface.
Zhonghua Zheng, Matthew West, Lei Zhao, Po-Lun Ma, Xiaohong Liu, and Nicole Riemer
Atmos. Chem. Phys., 21, 17727–17741, https://doi.org/10.5194/acp-21-17727-2021, https://doi.org/10.5194/acp-21-17727-2021, 2021
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Aerosol mixing state is an important emergent property that affects aerosol radiative forcing and aerosol–cloud interactions, but it has not been easy to constrain this property globally. We present a framework for evaluating the error in aerosol mixing state induced by aerosol representation assumptions, which is one of the important contributors to structural uncertainty in aerosol models. Our study provides insights into potential improvements to model process representation for aerosols.
Ksakousti Skyllakou, Pablo Garcia Rivera, Brian Dinkelacker, Eleni Karnezi, Ioannis Kioutsioukis, Carlos Hernandez, Peter J. Adams, and Spyros N. Pandis
Atmos. Chem. Phys., 21, 17115–17132, https://doi.org/10.5194/acp-21-17115-2021, https://doi.org/10.5194/acp-21-17115-2021, 2021
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Significant reductions in pollutant emissions took place in the US from 1990 to 2010. The reductions in sulfur dioxide emissions from electric-generating units have dominated the reductions in fine particle mass. The reductions in transportation emissions have led to a 30 % reduction of elemental concentrations and of organic particulate matter by a factor of 3. On the other hand, changes in biomass burning and biogenic secondary organic aerosol have been modest.
Nønne L. Prisle
Atmos. Chem. Phys., 21, 16387–16411, https://doi.org/10.5194/acp-21-16387-2021, https://doi.org/10.5194/acp-21-16387-2021, 2021
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A mass-based Gibbs adsorption model is presented to enable predictive Köhler calculations of droplet growth and activation with considerations of surface partitioning, surface tension, and non-ideal water activity for chemically complex and unresolved surface active aerosol mixtures, including actual atmospheric samples. The model is used to calculate cloud condensation nuclei (CCN) activity of aerosol particles comprising strongly surface-active model atmospheric humic-like substances (HULIS).
Ruqian Miao, Qi Chen, Manish Shrivastava, Youfan Chen, Lin Zhang, Jianlin Hu, Yan Zheng, and Keren Liao
Atmos. Chem. Phys., 21, 16183–16201, https://doi.org/10.5194/acp-21-16183-2021, https://doi.org/10.5194/acp-21-16183-2021, 2021
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We apply process-based and observation-constrained schemes to simulate organic aerosol in China and conduct comprehensive model–observation comparisons. The results show that anthropogenic semivolatile and intermediate-volatility organic compounds (SVOCs and IVOCs) are the main sources of secondary organic aerosol (SOA) in polluted regions, for which the residential sector is perhaps the predominant contributor. The hydroxyl radical level is also important for SOA modeling in polluted regions.
Yuqiang Zhang, Drew Shindell, Karl Seltzer, Lu Shen, Jean-Francois Lamarque, Qiang Zhang, Bo Zheng, Jia Xing, Zhe Jiang, and Lei Zhang
Atmos. Chem. Phys., 21, 16051–16065, https://doi.org/10.5194/acp-21-16051-2021, https://doi.org/10.5194/acp-21-16051-2021, 2021
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In this study, we use a global chemical transport model to simulate the effects on global air quality and human health due to emission changes in China from 2010 to 2017. By performing sensitivity analysis, we found that the air pollution control policies not only decrease the air pollutant concentration but also bring significant co-benefits in air quality to downwind regions. The benefits for the improved air pollution are dominated by PM2.5.
Anthony C. Jones, Adrian Hill, Samuel Remy, N. Luke Abraham, Mohit Dalvi, Catherine Hardacre, Alan J. Hewitt, Ben Johnson, Jane P. Mulcahy, and Steven T. Turnock
Atmos. Chem. Phys., 21, 15901–15927, https://doi.org/10.5194/acp-21-15901-2021, https://doi.org/10.5194/acp-21-15901-2021, 2021
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Ammonium nitrate is hard to model because it forms and evaporates rapidly. One approach is to relate its equilibrium concentration to temperature, humidity, and the amount of nitric acid and ammonia gases. Using this approach, we limit the rate at which equilibrium is reached using various condensation rates in a climate model. We show that ammonium nitrate concentrations are highly sensitive to the condensation rate. Our results will help improve the representation of nitrate in climate models.
Shuping Zhang, Golam Sarwar, Jia Xing, Biwu Chu, Chaoyang Xue, Arunachalam Sarav, Dian Ding, Haotian Zheng, Yujing Mu, Fengkui Duan, Tao Ma, and Hong He
Atmos. Chem. Phys., 21, 15809–15826, https://doi.org/10.5194/acp-21-15809-2021, https://doi.org/10.5194/acp-21-15809-2021, 2021
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Six heterogeneous HONO chemistry updates in CMAQ significantly improve HONO concentration. HONO production is primarily controlled by the heterogeneous reactions on ground and aerosol surfaces during haze. Additional HONO chemistry updates increase OH and production of secondary aerosols: sulfate, nitrate, and SOA.
Vlassis A. Karydis, Alexandra P. Tsimpidi, Andrea Pozzer, and Jos Lelieveld
Atmos. Chem. Phys., 21, 14983–15001, https://doi.org/10.5194/acp-21-14983-2021, https://doi.org/10.5194/acp-21-14983-2021, 2021
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Aerosol particle pH is well-buffered by alkaline compounds, notably NH3 and crustal elements. NH3 is found to supply remarkable buffering capacity on a global scale, from the polluted continents to the remote oceans. Potential future changes in agricultural NH3 must be accompanied by strong reductions of SO2 and NOx to avoid particles becoming highly acidic, with implications for human health (aerosol toxicity), ecosystems (acid deposition), clouds, and climate (aerosol hygroscopicity).
Lili Ren, Yang Yang, Hailong Wang, Pinya Wang, Lei Chen, Jia Zhu, and Hong Liao
Atmos. Chem. Phys., 21, 15431–15445, https://doi.org/10.5194/acp-21-15431-2021, https://doi.org/10.5194/acp-21-15431-2021, 2021
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Due to the COVID-19 pandemic, human activities were strictly restricted in China. Even though anthropogenic aerosol emissions largely decreased, haze events still occurred. Our results shows that PM2.5 over the North China Plain is largely contributed by local sources. For other regions in China, PM2.5 is largely contributed from nonlocal sources. As emission reduction is a future goal, aerosol long-range transport and unfavorable meteorology are increasingly important to air quality.
Mengmeng Li, Zihan Zhang, Quan Yao, Tijian Wang, Min Xie, Shu Li, Bingliang Zhuang, and Yong Han
Atmos. Chem. Phys., 21, 15135–15152, https://doi.org/10.5194/acp-21-15135-2021, https://doi.org/10.5194/acp-21-15135-2021, 2021
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We establish the nonlinear responses between nitrate and NOx in China. Reduction of NOx results in linearly lower nitrate in summer–autumn whereas an increase of winter nitrate until an inflexion point at 40–50 % reduction due to the excess oxidants. NH3 and VOCs are effective in controlling nitrate pollution, whereas decreasing the SO2 and NOx emissions may have counterintuitive effects on nitrate aerosols. This paper helps understand the nonlinear aerosol and photochemistry feedback.
Deepchandra Srivastava, Jingsha Xu, Tuan V. Vu, Di Liu, Linjie Li, Pingqing Fu, Siqi Hou, Natalia Moreno Palmerola, Zongbo Shi, and Roy M. Harrison
Atmos. Chem. Phys., 21, 14703–14724, https://doi.org/10.5194/acp-21-14703-2021, https://doi.org/10.5194/acp-21-14703-2021, 2021
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This study presents the source apportionment of PM2.5 performed by positive matrix factorization (PMF) at urban and rural sites in Beijing. These factors are interpreted as traffic emissions, biomass burning, road and soil dust, coal and oil combustion, and secondary inorganics. PMF failed to resolve some sources identified by CMB and AMS and appears to overestimate the dust sources. Comparison with earlier PMF studies from the Beijing area highlights inconsistent findings using this method.
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Short summary
Global lifetimes and concentrations of gaseous methylamines (MMA, DMA, and TMA) have been simulated.
Oxidation and aerosol uptakes are dominant sinks for these methylamines. The oxidation alone leads to their lifetimes of 5-10h in most parts of low and middle latitude regions. The uptake by secondary species can shorten their lifetime to as low as 1-2h over central Europe, eastern Asia, and the eastern US.
The modeled concentrations are substantially lower than observed values available.
Global lifetimes and concentrations of gaseous methylamines (MMA, DMA, and TMA) have been...
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