Articles | Volume 21, issue 8
https://doi.org/10.5194/acp-21-6221-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-21-6221-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Influence of atmospheric conditions on the role of trifluoroacetic acid in atmospheric sulfuric acid–dimethylamine nucleation
Key Laboratory of Cluster Science, Ministry of Education of China, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing 100081, China
Fangqun Yu
Atmospheric Sciences Research Center, University at Albany, Albany, New York 12203, USA
Kaipeng Tu
Key Laboratory of Cluster Science, Ministry of Education of China, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing 100081, China
Zhi Yang
Key Laboratory of Cluster Science, Ministry of Education of China, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing 100081, China
Key Laboratory of Cluster Science, Ministry of Education of China, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing 100081, China
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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.
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This study explores the effect of pyruvic acid (PA) both in the SO3 hydrolysis and in sulfuric-acid-based aerosol formation. Results show that in dry and polluted areas, PA-catalyzed SO3 hydrolysis is about 2 orders of magnitude more efficient at forming sulfuric acid than the water-catalyzed reaction. Moreover, PA can effectively enhance the ternary SA-PA-NH3 particle formation rate by up to 4.7×102 relative to the binary SA-NH3 particle formation rate at cold temperatures.
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Gongda Lu, Eloise A. Marais, Tuan V. Vu, Jingsha Xu, Zongbo Shi, James D. Lee, Qiang Zhang, Lu Shen, Gan Luo, and Fangqun Yu
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Revised manuscript not accepted
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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.
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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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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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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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
Short summary
Short summary
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.
F. Yu and G. Luo
Atmos. Chem. Phys., 14, 12455–12464, https://doi.org/10.5194/acp-14-12455-2014, https://doi.org/10.5194/acp-14-12455-2014, 2014
Short summary
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.
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
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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.
Trifluoroacetic acid (TFA) was previously proved to participate in sulfuric acid...
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