Research article
11 Feb 2022
Research article
| 11 Feb 2022
The number fraction of iron-containing particles affects OH, HO2 and H2O2 budgets in the atmospheric aqueous phase
Amina Khaled et al.
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Minghui Zhang, Amina Khaled, Pierre Amato, Anne-Marie Delort, and Barbara Ervens
Atmos. Chem. Phys., 21, 3699–3724, https://doi.org/10.5194/acp-21-3699-2021, https://doi.org/10.5194/acp-21-3699-2021, 2021
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Although primary biological aerosol particles (PBAPs, bioaerosols) represent a small fraction of total atmospheric aerosol burden, they might affect climate and public health. We summarize which PBAP properties are important to affect their inclusion in clouds and interaction with light and might also affect their residence time and transport in the atmosphere. Our study highlights that not only chemical and physical but also biological processes can modify these physicochemical properties.
Amina Khaled, Minghui Zhang, Pierre Amato, Anne-Marie Delort, and Barbara Ervens
Atmos. Chem. Phys., 21, 3123–3141, https://doi.org/10.5194/acp-21-3123-2021, https://doi.org/10.5194/acp-21-3123-2021, 2021
Saly Jaber, Muriel Joly, Maxence Brissy, Martin Leremboure, Amina Khaled, Barbara Ervens, and Anne-Marie Delort
Biogeosciences, 18, 1067–1080, https://doi.org/10.5194/bg-18-1067-2021, https://doi.org/10.5194/bg-18-1067-2021, 2021
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Our study is of interest to atmospheric scientists and environmental microbiologists, as we show that clouds can be considered a medium where bacteria efficiently degrade and transform amino acids, in competition with chemical processes. As current atmospheric multiphase models are restricted to chemical degradation of organic compounds, our conclusions motivate further model development.
Ramon Campos Braga, Barbara Ervens, Daniel Rosenfeld, Meinrat O. Andreae, Jan-David Förster, Daniel Fütterer, Lianet Hernández Pardo, Bruna A. Holanda, Tina Jurkat-Witschas, Ovid O. Krüger, Oliver Lauer, Luiz A. T. Machado, Christopher Pöhlker, Daniel Sauer, Christiane Voigt, Adrian Walser, Manfred Wendisch, Ulrich Pöschl, and Mira L. Pöhlker
Atmos. Chem. Phys., 21, 17513–17528, https://doi.org/10.5194/acp-21-17513-2021, https://doi.org/10.5194/acp-21-17513-2021, 2021
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Interactions of aerosol particles with clouds represent a large uncertainty in estimates of climate change. Properties of aerosol particles control their ability to act as cloud condensation nuclei. Using aerosol measurements in the Amazon, we performed model studies to compare predicted and measured cloud droplet number concentrations at cloud bases. Our results confirm previous estimates of particle hygroscopicity in this region.
Ramon Campos Braga, Daniel Rosenfeld, Ovid O. Krüger, Barbara Ervens, Bruna A. Holanda, Manfred Wendisch, Trismono Krisna, Ulrich Pöschl, Meinrat O. Andreae, Christiane Voigt, and Mira L. Pöhlker
Atmos. Chem. Phys., 21, 14079–14088, https://doi.org/10.5194/acp-21-14079-2021, https://doi.org/10.5194/acp-21-14079-2021, 2021
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Quantifying the precipitation within clouds is crucial for our understanding of the Earth's hydrological cycle. Using in situ measurements of cloud and rain properties over the Amazon Basin and Atlantic Ocean, we show here a linear relationship between the effective radius (re) and precipitation water content near the tops of convective clouds for different pollution states and temperature levels. Our results emphasize the role of re to determine both initiation and amount of precipitation.
Mira L. Pöhlker, Minghui Zhang, Ramon Campos Braga, Ovid O. Krüger, Ulrich Pöschl, and Barbara Ervens
Atmos. Chem. Phys., 21, 11723–11740, https://doi.org/10.5194/acp-21-11723-2021, https://doi.org/10.5194/acp-21-11723-2021, 2021
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Clouds cool our atmosphere. The role of small aerosol particles in affecting them represents one of the largest uncertainties in current estimates of climate change. Traditionally it is assumed that cloud droplets only form particles of diameters ~ 100 nm (
accumulation mode). Previous studies suggest that this can also occur in smaller particles (
Aitken mode). Our study provides a general framework to estimate under which aerosol and cloud conditions Aitken mode particles affect clouds.
Minghui Zhang, Amina Khaled, Pierre Amato, Anne-Marie Delort, and Barbara Ervens
Atmos. Chem. Phys., 21, 3699–3724, https://doi.org/10.5194/acp-21-3699-2021, https://doi.org/10.5194/acp-21-3699-2021, 2021
Short summary
Short summary
Although primary biological aerosol particles (PBAPs, bioaerosols) represent a small fraction of total atmospheric aerosol burden, they might affect climate and public health. We summarize which PBAP properties are important to affect their inclusion in clouds and interaction with light and might also affect their residence time and transport in the atmosphere. Our study highlights that not only chemical and physical but also biological processes can modify these physicochemical properties.
Amina Khaled, Minghui Zhang, Pierre Amato, Anne-Marie Delort, and Barbara Ervens
Atmos. Chem. Phys., 21, 3123–3141, https://doi.org/10.5194/acp-21-3123-2021, https://doi.org/10.5194/acp-21-3123-2021, 2021
Saly Jaber, Muriel Joly, Maxence Brissy, Martin Leremboure, Amina Khaled, Barbara Ervens, and Anne-Marie Delort
Biogeosciences, 18, 1067–1080, https://doi.org/10.5194/bg-18-1067-2021, https://doi.org/10.5194/bg-18-1067-2021, 2021
Short summary
Short summary
Our study is of interest to atmospheric scientists and environmental microbiologists, as we show that clouds can be considered a medium where bacteria efficiently degrade and transform amino acids, in competition with chemical processes. As current atmospheric multiphase models are restricted to chemical degradation of organic compounds, our conclusions motivate further model development.
Saly Jaber, Audrey Lallement, Martine Sancelme, Martin Leremboure, Gilles Mailhot, Barbara Ervens, and Anne-Marie Delort
Atmos. Chem. Phys., 20, 4987–4997, https://doi.org/10.5194/acp-20-4987-2020, https://doi.org/10.5194/acp-20-4987-2020, 2020
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Current atmospheric multiphase models do not include biotransformations of organic compounds by bacteria, although many previous studies of our and other research groups have shown microbial activity in cloud water. The current lab/model study shows that for water-soluble aromatic compounds, biodegradation by bacteria may be as efficient as chemical reactions in cloud water.
Barbara Ervens and Pierre Amato
Atmos. Chem. Phys., 20, 1777–1794, https://doi.org/10.5194/acp-20-1777-2020, https://doi.org/10.5194/acp-20-1777-2020, 2020
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Bacteria in the atmosphere are important due to their potential adverse health effects and as initiators of ice cloud formation. Observational studies suggest that bacterial cells grow and multiply in clouds and also consume organic compounds.
We estimate the role of microbial processes in the atmosphere for (i) the increase in biological aerosol mass by cell growth and multiplication and (ii) the sink strength of organics in clouds as a loss process in addition to chemical reactions.
Barbara Ervens, Armin Sorooshian, Abdulmonam M. Aldhaif, Taylor Shingler, Ewan Crosbie, Luke Ziemba, Pedro Campuzano-Jost, Jose L. Jimenez, and Armin Wisthaler
Atmos. Chem. Phys., 18, 16099–16119, https://doi.org/10.5194/acp-18-16099-2018, https://doi.org/10.5194/acp-18-16099-2018, 2018
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The paper presents a new framework that can be used to identify emission scenarios in which aerosol populations are most likely modified by chemical processes in clouds. We show that in neither very polluted nor in very clean air masses is this the case. Only if the ratio of possible aerosol mass precursors (sulfur dioxide, some organics) and preexisting aerosol mass is sufficiently high will aerosol particles show substantially modified physicochemical properties upon cloud processing.
B. Ervens, P. Renard, S. Tlili, S. Ravier, J.-L. Clément, and A. Monod
Atmos. Chem. Phys., 15, 9109–9127, https://doi.org/10.5194/acp-15-9109-2015, https://doi.org/10.5194/acp-15-9109-2015, 2015
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A detailed chemical mechanism is developed based on laboratory studies that predicts the formation of high molecular weight compounds in the aqueous phase of atmospheric aerosol particles. Model simulations using this mechanism for atmospheric conditions show that these pathways are likely not a substantial source of particle mass, unless unidentified precursors for these compounds exist that were not taken into account so far and/or the solubility of oxygen in aerosol water is overestimated.
B. Yuan, P. R. Veres, C. Warneke, J. M. Roberts, J. B. Gilman, A. Koss, P. M. Edwards, M. Graus, W. C. Kuster, S.-M. Li, R. J. Wild, S. S. Brown, W. P. Dubé, B. M. Lerner, E. J. Williams, J. E. Johnson, P. K. Quinn, T. S. Bates, B. Lefer, P. L. Hayes, J. L. Jimenez, R. J. Weber, R. Zamora, B. Ervens, D. B. Millet, B. Rappenglück, and J. A. de Gouw
Atmos. Chem. Phys., 15, 1975–1993, https://doi.org/10.5194/acp-15-1975-2015, https://doi.org/10.5194/acp-15-1975-2015, 2015
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In this work, secondary formation of formic acid at an urban site and a site in an oil and gas production region is studied. We investigated various gas phase formation pathways of formic acid, including those recently proposed, using a box model. The contributions from aerosol-related processes, fog events and air-snow exchange to formic acid are also quantified.
B. Ervens, Y. Wang, J. Eagar, W. R. Leaitch, A. M. Macdonald, K. T. Valsaraj, and P. Herckes
Atmos. Chem. Phys., 13, 5117–5135, https://doi.org/10.5194/acp-13-5117-2013, https://doi.org/10.5194/acp-13-5117-2013, 2013
Related subject area
Subject: Aerosols | Research Activity: Atmospheric Modelling | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
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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.
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.
Yao Ge, Massimo Vieno, David Stevenson, Peter Wind, and Mathew Heal
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-82, https://doi.org/10.5194/acp-2022-82, 2022
Revised manuscript accepted for ACP
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Reactive N and S gases and particle are critical determinants of air quality. We reports a comprehensive analysis of the concentrations, wet and dry deposition, fluxes and lifetimes of these species globally, and 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.
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.
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.
Hitoshi Matsui, Tatsuhiro Mori, Sho Ohata, Nobuhiro Moteki, Naga Oshima, Kumiko Goto-Azuma, Makoto Koike, and Yutaka Kondo
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-1091, https://doi.org/10.5194/acp-2021-1091, 2022
Revised manuscript accepted for ACP
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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.
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.
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.
Xinxin Ye, Pargoal Arab, Ravan Ahmadov, Eric James, Georg A. Grell, Bradley Pierce, Aditya Kumar, Paul Makar, Jack Chen, Didier Davignon, Greg R. Carmichael, Gonzalo Ferrada, Jeff McQueen, Jianping Huang, Rajesh Kumar, Louisa Emmons, Farren L. Herron-Thorpe, Mark Parrington, Richard Engelen, Vincent-Henri Peuch, Arlindo da Silva, Amber Soja, Emily Gargulinski, Elizabeth Wiggins, Johnathan W. Hair, Marta Fenn, Taylor Shingler, Shobha Kondragunta, Alexei Lyapustin, Yujie Wang, Brent Holben, David M. Giles, and Pablo E. Saide
Atmos. Chem. Phys., 21, 14427–14469, https://doi.org/10.5194/acp-21-14427-2021, https://doi.org/10.5194/acp-21-14427-2021, 2021
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Wildfire smoke has crucial impacts on air quality, while uncertainties in the numerical forecasts remain significant. We present an evaluation of 12 real-time forecasting systems. Comparison of predicted smoke emissions suggests a large spread in magnitudes, with temporal patterns deviating from satellite detections. The performance for AOD and surface PM2.5 and their discrepancies highlighted the role of accurately represented spatiotemporal emission profiles in improving smoke forecasts.
Huan Song, Keding Lu, Can Ye, Huabin Dong, Shule Li, Shiyi Chen, Zhijun Wu, Mei Zheng, Limin Zeng, Min Hu, and Yuanhang Zhang
Atmos. Chem. Phys., 21, 13713–13727, https://doi.org/10.5194/acp-21-13713-2021, https://doi.org/10.5194/acp-21-13713-2021, 2021
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Secondary sulfate aerosols are an important component of fine particles in severe air pollution events. We calculated the sulfate formation rates via a state-of-the-art multiphase model constrained to the observed values. We showed that transition metals in urban aerosols contribute significantly to sulfate formation during haze periods and thus play an important role in mitigation strategies and public health measures in megacities worldwide.
Emma Lumiaro, Milica Todorović, Theo Kurten, Hanna Vehkamäki, and Patrick Rinke
Atmos. Chem. Phys., 21, 13227–13246, https://doi.org/10.5194/acp-21-13227-2021, https://doi.org/10.5194/acp-21-13227-2021, 2021
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The study of climate change relies on climate models, which require an understanding of aerosol formation. We train a machine-learning model to predict the partitioning coefficients of atmospheric molecules, which govern condensation into aerosols. The model can make instant predictions based on molecular structures with accuracy surpassing that of standard computational methods. This will allow the screening of low-volatility molecules that contribute most to aerosol formation.
Yun Fat Lam, Chi Chiu Cheung, Xuguo Zhang, Joshua S. Fu, and Jimmy Chi Hung Fung
Atmos. Chem. Phys., 21, 12895–12908, https://doi.org/10.5194/acp-21-12895-2021, https://doi.org/10.5194/acp-21-12895-2021, 2021
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In recent years, air pollution forecasting has become an important municipal service of the government. In this study, a new spatial allocation method based on satellite remote sensing and GIS techniques was developed to address the spatial deficiency of industrial source emissions in China, providing a substantial improvement on NO2 and PM2.5 forecast for the Pearl River Delta/Greater Bay Area.
Camilla Geels, Morten Winther, Camilla Andersson, Jukka-Pekka Jalkanen, Jørgen Brandt, Lise M. Frohn, Ulas Im, Wing Leung, and Jesper H. Christensen
Atmos. Chem. Phys., 21, 12495–12519, https://doi.org/10.5194/acp-21-12495-2021, https://doi.org/10.5194/acp-21-12495-2021, 2021
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In this study, we set up new shipping emissions scenarios and use two chemistry transport models and a health assessment model to assess the development of air quality and related health impacts in the Nordic region. Shipping alone is associated with about 850 premature deaths during present-day conditions, decreasing to approximately 550–600 cases in the 2050 scenarios.
Sabrina Chee, Kelley Barsanti, James N. Smith, and Nanna Myllys
Atmos. Chem. Phys., 21, 11637–11654, https://doi.org/10.5194/acp-21-11637-2021, https://doi.org/10.5194/acp-21-11637-2021, 2021
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We explored molecular properties affecting atmospheric particle formation efficiency and derived a parameterization between particle formation rate and heterodimer concentration, which showed good agreement to previously reported experimental data. Considering the simplicity of calculating heterodimer concentration, this approach has potential to improve estimates of global cloud condensation nuclei in models that are limited by the computational expense of calculating particle formation rate.
Isaac Kwadjo Afreh, Bernard Aumont, Marie Camredon, and Kelley Claire Barsanti
Atmos. Chem. Phys., 21, 11467–11487, https://doi.org/10.5194/acp-21-11467-2021, https://doi.org/10.5194/acp-21-11467-2021, 2021
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This is the first mechanistic modeling study of secondary organic aerosol (SOA) from the understudied monoterpene, camphene. The semi-explicit chemical model GECKO-A predicted camphene SOA yields that were ~2 times α-pinene. Using 50/50 α-pinene + limonene as a surrogate for camphene increased predicted SOA mass from biomass burning fuels by up to ~100 %. The accurate representation of camphene in air quality models can improve predictions of SOA when camphene is a dominant monoterpene.
Caterina Mogno, Paul I. Palmer, Christoph Knote, Fei Yao, and Timothy J. Wallington
Atmos. Chem. Phys., 21, 10881–10909, https://doi.org/10.5194/acp-21-10881-2021, https://doi.org/10.5194/acp-21-10881-2021, 2021
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We use a 3-D atmospheric chemistry model to investigate how seasonal emissions sources and meteorological conditions affect the surface distribution of fine particulate matter (PM2.5) and organic aerosol (OA) over the Indo-Gangetic Plain. We find that all seasonal mean values of PM2.5 still exceed safe air quality levels, with human emissions contributing to PM2.5 all year round, open fires during post- and pre-monsoon, and biogenic emissions during monsoon. OA contributes up to 30 % to PM2.5.
Liangying Zeng, Yang Yang, Hailong Wang, Jing Wang, Jing Li, Lili Ren, Huimin Li, Yang Zhou, Pinya Wang, and Hong Liao
Atmos. Chem. Phys., 21, 10745–10761, https://doi.org/10.5194/acp-21-10745-2021, https://doi.org/10.5194/acp-21-10745-2021, 2021
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Using an aerosol–climate model, the impacts of El Niño with different durations on aerosols in China are examined. The modulation on aerosol concentrations and haze days by short-duration El Niño events is 2–3 times more than that by long-duration El Niño events in China. The frequency of short-duration El Niño has been increasing significantly in recent decades, suggesting that El Niño events have exerted increasingly intense modulation on aerosol pollution in China over the past few decades.
Cited articles
Al-Abadleh, H. A.: Review of the bulk and surface chemistry of iron in
atmospherically relevant systems containing humic-like substances, RSC
Adv., 5, 45785–45811, https://doi.org/10.1039/C5RA03132J, 2015. a
Alexander, B., Park, R. J., Jacob, D. J., and Gong, S.: Transition
metal-catalyzed oxidation of atmospheric sulfur: Global implications for the
sulfur budget, J. Geophys. Res.-Atmos., 114, D02309,
https://doi.org/10.1029/2008jd010486, 2009. a
Arangio, A. M., Slade, J. H., Berkemeier, T., Pöschl, U., Knopf, D. A.,
and Shiraiwa, M.: Multiphase Chemical Kinetics of OH Radical Uptake by
Molecular Organic Markers of Biomass Burning Aerosols: Humidity and
Temperature Dependence, Surface Reaction, and Bulk Diffusion, J.
Phys. Chem. A, 119, 4533–4544, https://doi.org/10.1021/jp510489z, 2015. a
Arangio, A. M., Tong, H., Socorro, J., Pöschl, U., and Shiraiwa, M.:
Quantification of environmentally persistent free radicals and reactive
oxygen species in atmospheric aerosol particles, Atmos. Chem. Phys., 16,
13105–13119, https://doi.org/10.5194/acp-16-13105-2016, 2016. a
Barth, M. C., Ervens, B., Herrmann, H., Tilgner, A., McNeill, V. F., Tsui,
W. G., Deguillaume, L., Chaumerliac, N., Carlton, A. G., and Lance, S.: Box
Model Intercomparison of Cloud Chemistry, J. Geophys. Res.-Atmos., 126, e2021JD035486, https://doi.org/10.1029/2021JD035486, 2021. a, b
Bedjanian, Y., Lelièvre, S., and Le Bras, G.: Experimental study of
the interaction of HO2 radicals with soot surface, Phys. Chem. Chem. Phys.,
7, 334–341, https://doi.org/10.1039/B414217A, 2005. a
Bertram, A. K., Ivanov, A. V., Hunter, M., Molina, L. T., and Molina, M. J.:
The reaction probability of OH on Organic Surfaces of Tropospheric
Interest, J. Phys. Chem. A, 105, 9415–9421,
https://doi.org/10.1021/jp0114034, 2001. a
Bianchini, R. H., Tesa-Serrate, M. A., Costen, M. L., and McKendrick, K. G.:
Collision-Energy Dependence of the Uptake of Hydroxyl Radicals at
Atmospherically Relevant Liquid Surfaces, J. Phys. Chem.
C, 122, 6648–6660, https://doi.org/10.1021/acs.jpcc.7b12574, 2018. a
Bianco, A., Passananti, M., Perroux, H., Voyard, G., Mouchel-Vallon, C.,
Chaumerliac, N., Mailhot, G., Deguillaume, L., and Brigante, M.: A better
understanding of hydroxyl radical photochemical sources in cloud waters
collected at the puy de Dôme station – experimental versus modelled
formation rates, Atmos. Chem. Phys., 15, 9191–9202,
https://doi.org/10.5194/acp-15-9191-2015, 2015. a
Chan, M. N., Zhang, H., Goldstein, A. H., and Wilson, K. R.: Role of Water and
Phase in the Heterogeneous Oxidation of Solid and Aqueous Succinic Acid
Aerosol by Hydroxyl Radicals, J. Phys. Chem. C, 118,
28978–28992, https://doi.org/10.1021/jp5012022, 2014. a
Chang, J. S., Brost, R. A., Isaksen, I. S. A., Madronich, S., Middleton, P.,
Stockwell, W. R., and Walcek, C. J.: A three-dimensional Eulerian acid
deposition model: Physical concepts and formulation, J. Geophys. Res.-Atmos., 92, 14681–14700, https://doi.org/10.1029/JD092iD12p14681, 1987. a
Charrier, J. G. and Anastasio, C.: On dithiothreitol (DTT) as a measure of
oxidative potential for ambient particles: evidence for the importance of
soluble transition metals, Atmos. Chem. Phys., 12,
9321–9333, https://doi.org/10.5194/acp-12-9321-2012, 2012. a
Charrier, J. G., Richards-Henderson, N. K., Bein, K. J., McFall, A. S., Wexler, A. S., and Anastasio, C.: Oxidant production from source-oriented particulate matter – Part 1: Oxidative potential using the dithiothreitol (DTT) assay, Atmos. Chem. Phys., 15, 2327–2340, https://doi.org/10.5194/acp-15-2327-2015, 2015. a
Che, D. L., Smith, J. D., Leone, S. R., Ahmed, M., and Wilson, K. R.:
Quantifying the reactive uptake of OH by organic aerosols in a continuous
flow stirred tank reactor, Phys. Chem. Chem. Phys., 11, 7885–7895,
https://doi.org/10.1039/B904418C, 2009. a
Choël, M., Deboudt, K., Flament, P., Aimoz, L., and Mériaux, X.:
Single-particle analysis of atmospheric aerosols at Cape Gris-Nez, English
Channel: Influence of steel works on iron apportionment, Atmos.
Environ., 41, 2820–2830, https://doi.org/10.1016/j.atmosenv.2006.11.038, 2007. a
Christian, K. E., Brune, W. H., and Mao, J.: Global sensitivity analysis of
the GEOS-Chem chemical transport model: ozone and hydrogen oxides during
ARCTAS (2008), Atmos. Chem. Phys., 17, 3769–3784,
https://doi.org/10.5194/acp-17-3769-2017, 2017. a
Cini, R., Prodi, F., Santachiara, G., Porcu, F., Bellandi, S., Stortini, A.,
Oppo, C., Udisti, R., and Pantani, F.: Chemical characterization of cloud
episodes at a ridge site in Tuscan Appennines, Italy, Atmos. Res.,
61, 311–334, https://doi.org/10.1016/S0169-8095(01)00139-9, 2002. a
Cooper, P. L. and Abbatt, J. P. D.: Heterogeneous Interactions of OH and
HO2 Radicals with Surfaces Characteristic of Atmospheric
Particulate Matter, J. Phys. Chem., 100, 2249–2254,
https://doi.org/10.1021/jp952142z, 1996. a
Ervens, B.: Modeling the Processing of Aerosol and Trace Gases in Clouds and
Fogs, Chem. Rev., 115, 4157–4198, https://doi.org/10.1021/cr5005887, 2015. a, b, c
Ervens, B.: Model output, Khaled et al., Iron distribution in the aqueous phase, Zenodo [data set], https://doi.org/10.5281/zenodo.5829360, 2022. a
Ervens, B., George, C., Williams, J. E., Buxton, G. V., Salmon, G. A., Bydder,
M., Wilkinson, F., Dentener, F., Mirabel, P., Wolke, R., and Herrmann, H.:
CAPRAM2.4 (MODAC mechanism): An extended and condensed tropospheric aqueous
phase mechanism and its application, J. Geophys. Res., 108, 4426, https://doi.org/10.1029/2002JD002202, 2003. a, b, c, d, e
Ervens, B., Carlton, A. G., Turpin, B. J., Altieri, K. E., Kreidenweis, S. M.,
and Feingold, G.: Secondary organic aerosol yields from cloud-processing of
isoprene oxidation products, Geophys. Res. Lett., 35, L02816,
https://doi.org/10.1029/2007gl031828, 2008. a
Ervens, B., Turpin, B. J., and Weber, R. J.: Secondary organic aerosol formation in cloud droplets and aqueous particles (aqSOA): a review of laboratory, field and model studies, Atmos. Chem. Phys., 11, 11069–11102, https://doi.org/10.5194/acp-11-11069-2011, 2011. a
Ervens, B., Sorooshian, A., Lim, Y. B., and Turpin, B. J.: Key parameters
controlling OH-initiated formation of secondary organic aerosol in the
aqueous phase (aqSOA), J. Geophys. Res.-Atmos., 119, 3997–4016,
https://doi.org/10.1002/2013JD021021, 2014. a, b
Fang, T., Verma, V., Bates, J. T., Abrams, J., Klein, M., Strickland, M. J., Sarnat, S. E., Chang, H. H., Mulholland, J. A., Tolbert, P. E., Russell, A. G., and Weber, R. J.: Oxidative potential of ambient water-soluble PM2.5 in the southeastern United States: contrasts in sources and health associations between ascorbic acid (AA) and dithiothreitol (DTT) assays, Atmos. Chem. Phys., 16, 3865–3879, https://doi.org/10.5194/acp-16-3865-2016, 2016. a
Fang, T., Guo, H., Zeng, L., Verma, V., Nenes, A., and Weber, R. J.: Highly
Acidic Ambient Particles, Soluble Metals, and Oxidative Potential: A Link
between Sulfate and Aerosol Toxicity, Environ. Sci. Technol.,
51, 2611–2620, https://doi.org/10.1021/acs.est.6b06151, 2017. a
Fomba, K. W., van Pinxteren, D., Müller, K., Iinuma, Y., Lee, T.,
Collett Jr., J. L., and Herrmann, H.: Trace metal characterization of
aerosol particles and cloud water during HCCT 2010, Atmos. Chem.
Phys., 15, 8751–8765, https://doi.org/10.5194/acp-15-8751-2015, 2015. a, b
Furutani, H., Jung, J., Miura, K., Takami, A., Kato, S., Kajii, Y., and
Uematsu, M.: Single-particle chemical characterization and source
apportionment of iron-containing atmospheric aerosols in Asian outflow, J.
Geophys. Res.-Atmos., 116, D18204, https://doi.org/10.1029/2011jd015867, 2011. a
George, I. J., Vlasenko, A., Slowik, J. G., Broekhuizen, K., and Abbatt, J.
P. D.: Heterogeneous oxidation of saturated organic aerosols by hydroxyl
radicals: uptake kinetics, condensed-phase products, and particle size
change, Atmos. Chem. Phys., 7, 4187–4201,
https://doi.org/10.5194/acp-7-4187-2007, 2007. a
Guo, J., Wang, Z., Wang, T., and Zhang, X.: Theoretical evaluation of
different factors affecting the HO2 uptake coefficient driven by
aqueous-phase first-order loss reaction, Sci. Total Environ.,
683, 146–153, https://doi.org/10.1016/j.scitotenv.2019.05.237, 2019. a
Haggerstone, A.-L., Carpenter, L. J., N., C., and McFiggans, G.: Improved
model predictions of
HO2 with gas to
particle mass transfer rates calculated using aerosol number size
distributions, J. Geophys. Res., 110, , D04303, https://doi.org/10.1029/2004JD005282, 2005. a
Hanson, D. R., Burkholder, J. B., Howard, C. J., and Ravishankara, A. R.:
Measurement of hydroxyl and hydroperoxy radical uptake coefficients on water
and sulfuric acid surfaces, J. Phys. Chem., 96, 4979–4985,
https://doi.org/10.1021/j100191a046, 1992. a, b
Hasson, A. S. and Paulson, S. E.: An investigation of the relationship between
gas-phase and aerosol borne hydroperoxides in urban air, J. Aerosol Sci.,
34, 459–468, https://doi.org/10.1016/S0021-8502(03)00002-8, 2003. a, b
Herrmann, H., Ervens, B., Jacobi, H.-W., Wolke, R., Nowacki, P., and Zellner,
R.: CAPRAM2.3: A Chemical Aqueous Phase Radical Mechanism for Tropospheric
Chemistry, J. Atmos. Chem., 36, 231–284,
2000. a
Houle, F. A., Hinsberg, W. D., and Wilson, K. R.: Oxidation of a model alkane
aerosol by OH radical: the emergent nature of reactive uptake, Phys. Chem.
Chem. Phys., 17, 4412–4423, https://doi.org/10.1039/C4CP05093B, 2015. a, b
Ingall, E. D., Feng, Y., Longo, A. F., Lai, B., Shelley, R. U., Landing, W. M.,
Morton, P. L., Nenes, A., Mihalopoulos, N., Violaki, K., Gao, Y., Sahai, S.,
and Castorina, E.: Enhanced Iron Solubility at Low pH in Global Aerosols, Atmosphere, 9, 201,
https://doi.org/10.3390/atmos9050201, 2018. a, b, c
Jacob, D. J.: Heterogeneous chemistry and tropospheric ozone, Atmos. Environ.,
34, 2131–2159, https://doi.org/10.1016/S1352-2310(99)00462-8, 2000. a, b
Khaled, A., Zhang, M., Amato, P., Delort, A.-M., and Ervens, B.:
Biodegradation by bacteria in clouds: an underestimated sink for some
organics in the atmospheric multiphase system, Atmos. Chem.
Phys., 21, 3123–3141, https://doi.org/10.5194/acp-21-3123-2021, 2021. a
Lakey, P. S. J., George, I. J., Whalley, L. K., Baeza-Romero, M. T., and Heard,
D. E.: Measurements of the HO2 Uptake Coefficients onto Single Component
Organic Aerosols, Environ. Sci. Technol., 49, 4878–4885,
https://doi.org/10.1021/acs.est.5b00948, 2015. a, b, c
Lakey, P. S. J., Berkemeier, T., Krapf, M., Dommen, J., Steimer, S. S.,
Whalley, L. K., Ingham, T., Baeza-Romero, M. T., Pöschl, U., Shiraiwa,
M., Ammann, M., and Heard, D. E.: The effect of viscosity and diffusion on
the HO2 uptake by sucrose and secondary organic aerosol particles, Atmos.
Chem. Phys., 16, 13035–13047, https://doi.org/10.5194/acp-16-13035-2016, 2016. a
Li, J. and Knopf, D. A.: Representation of Multiphase OH Oxidation of
Amorphous Organic Aerosol for Tropospheric Conditions, Environ. Sci. Technol., 55, 7266–7275, https://doi.org/10.1021/acs.est.0c07668, 2021. a
Li, K., Jacob, D. J., Liao, H., Shen, L., Zhang, Q., and Bates, K. H.:
Anthropogenic drivers of 2013–2017 trends in summer surface ozone in
China, P. Natl. Acad. Sci. USA, 116, 422–427,
https://doi.org/10.1073/pnas.1812168116, 2019. a
Luo, C., Mahowald, N. M., Meskhidze, N., Chen, Y., Siefert, R. L., Baker,
A. R., and Johansen, A. M.: Estimation of iron solubility from observations
and a global aerosol model, J. Geophys. Res.-Atmos.,
110, D23307, https://doi.org/10.1029/2005JD006059, 2005. a, b
Lyu, Y., Guo, H., Cheng, T., and Li, X.: Particle Size Distributions of
Oxidative Potential of Lung-Deposited Particles: Assessing Contributions from
Quinones and Water-Soluble Metals, Environ. Sci. Technol.,
52, 6592–6600, https://doi.org/10.1021/acs.est.7b06686, 2018. a
Macintyre, H. L. and Evans, M. J.: Parameterisation and impact of aerosol
uptake of HO2 on a global tropospheric model, Atmos. Chem.
Phys., 11, 10965–10974, https://doi.org/10.5194/acp-11-10965-2011, 2011. a
Madronich, S. and Calvert, J. G.: The NCAR Master Mechanism of the Gas Phase
Chemistry – Version 2.0, Tech. Rep., No. NCAR/TN-333+STR, University
Corporation for Atmospheric Research, https://doi.org/10.5065/D6HD7SKH, 1989. a
Mao, J., Fan, S., Jacob, D. J., and Travis, K. R.: Radical loss in the atmosphere from Cu-Fe redox coupling in aerosols, Atmos. Chem. Phys., 13, 509–519, https://doi.org/10.5194/acp-13-509-2013, 2013. a, b, c, d
Mao, J., Fan, S., and Horowitz, L. W.: Soluble Fe in Aerosols Sustained by
Gaseous HO2 Uptake, Environ. Sci. Technol. Lett., 4,
98–104, https://doi.org/10.1021/acs.estlett.7b00017, 2017. a, b, c
Matthews, P. S. J., Baeza-Romero, M. T., Whalley, L. K., and Heard, D. E.:
Uptake of HO2 radicals onto Arizona test dust particles
using an aerosol flow tube, Atmos. Chem. Phys., 14,
7397–7408, https://doi.org/10.5194/acp-14-7397-2014, 2014. a
Moffet, R. C., Furutani, H., Rödel, T. C., Henn, T. R., Sprau, P. O.,
Laskin, A., Uematsu, M., and Gilles, M. K.: Iron speciation and mixing in
single aerosol particles from the Asian continental outflow, J.
Geophys. Res.-Atmos., 117, D07204, https://doi.org/10.1029/2011JD016746, 2012. a
Molina, C., Toro A., R., Manzano, C. A., Canepari, S., Massimi, L., and
Leiva-Guzmán, M. A.: Airborne Aerosols and Human Health: Leapfrogging
from Mass Concentration to Oxidative Potential, Atmosphere, 11, 917, https://doi.org/10.3390/atmos11090917,
2020. a, b
Moon, D. R., Taverna, G. S., Anduix-Canto, C., Ingham, T., Chipperfield, M. P.,
Seakins, P. W., Baeza-Romero, M.-T., and Heard, D. E.: Heterogeneous
reaction of HO2 with airborne TiO2
particles and its implication for climate change mitigation strategies,
Atmos. Chem. Phys., 18, 327–338,
https://doi.org/10.5194/acp-18-327-2018, 2018. a
Morita, A., Kanaya, Y., and Francisco, J. S.: Uptake of the HO2 radical by
water: Molecular dynamics calculations and their implications for atmospheric
modeling, J. Geophys. Res.-Atmos., 109, D09201,
https://doi.org/10.1029/2003jd004240, 2004. a
Myriokefalitakis, S., Ito, A., Kanakidou, M., Nenes, A., Krol, M. C., Mahowald,
N. M., Scanza, R. A., Hamilton, D. S., Johnson, M. S., Meskhidze, N., Kok,
J. F., Guieu, C., Baker, A. R., Jickells, T. D., Sarin, M. M., Bikkina, S.,
Shelley, R., Bowie, A., Perron, M. M. G., and Duce, R. A.: Reviews and
syntheses: the GESAMP atmospheric iron deposition model intercomparison
study, Biogeosciences, 15, 6659–6684, https://doi.org/10.5194/bg-15-6659-2018, 2018. a
Nathanson, G. M., Davidovits, P., Worsnop, D. R., and Kolb, C. E.: Dynamics
and Kinetics at the Gas-Liquid Interface, J. Phys. Chem., 100,
13007–13020, https://doi.org/10.1021/jp953548e, 1996. a, b
Pöschl, U. and Shiraiwa, M.: Multiphase Chemistry at the
Atmosphere–Biosphere Interface Influencing Climate and Public Health in the
Anthropocene, Chem. Rev., 115, 4440–4475, https://doi.org/10.1021/cr500487s,
2015. a
Pöschl, U., Rudich, Y., and Ammann, M.: Kinetic model framework for
aerosol and cloud surface chemistry and gas-particle interactions –
Part 1: General equations, parameters, and terminology, Atmos.
Chem. Phys., 7, 5989–6023, https://doi.org/10.5194/acp-7-5989-2007, 2007. a
Remorov, R. G., Gershenzon, Y. M., Molina, L. T., and Molina, M. J.: Kinetics
and Mechanism of HO2 Uptake on Solid NaCl, J. Phys. Chem.
A, 106, 4558–4565, https://doi.org/10.1021/jp013179o, 2002. a
Renbaum, L. H. and Smith, G. D.: Artifacts in measuring aerosol uptake kinetics: the roles of time, concentration and adsorption, Atmos. Chem. Phys., 11, 6881–6893, https://doi.org/10.5194/acp-11-6881-2011, 2011. a
Roeselová, M., Jungwirth, P., Tobias, D. J., and Gerber, R. B.: Impact,
Trapping, and Accommodation of Hydroxyl Radical and Ozone at Aqueous Salt
Aerosol Surfaces, A Molecular Dynamics Study, J. Phys.
Chem. B, 107, 12690–12699, https://doi.org/10.1021/jp030592i, 2003. a
Saffari, A., Daher, N., Shafer, M. M., Schauer, J. J., and Sioutas, C.: Global
Perspective on the Oxidative Potential of Airborne Particulate Matter: A
Synthesis of Research Findings, Environ. Sci. Technol., 48,
7576–7583, https://doi.org/10.1021/es500937x, 2014. a, b
Schwartz, S. E.: Mass-Transport Considerations Pertinent to Aqueous Phase
Reactions of Gases in Liquid-Water Clouds, in: Chemistry of Multiphase
Atmospheric Systems of Multiphase Atmospheric Systems, edited by: Jaeschke,
W., NATO ASI Series, Series G: Ecological Sciences, Berlin,
Heidelberg, Springer, 415–471, https://doi.org/10.1007/978-3-642-70627-1_16, 1986. a
Shahpoury, P., Zhang, Z. W., Arangio, A., Celo, V., Dabek-Zlotorzynska, E.,
Harner, T., and Nenes, A.: The influence of chemical composition, aerosol
acidity, and metal dissolution on the oxidative potential of fine particulate
matter and redox potential of the lung lining fluid, Environ.
Int., 148, 106343, https://doi.org/10.1016/j.envint.2020.106343, 2021. a
Slade, J. H. and Knopf, D. A.: Heterogeneous OH oxidation of biomass burning
organic aerosol surrogate compounds: assessment of volatilisation products
and the role of OH concentration on the reactive uptake kinetics, Phys.
Chem. Chem. Phys., 15, 5898–5915, https://doi.org/10.1039/C3CP44695F, 2013. a
Smith, J. D., Kroll, J. H., Cappa, C. D., Che, D. L., Liu, C. L., Ahmed, M.,
Leone, S. R., Worsnop, D. R., and Wilson, K. R.: The heterogeneous reaction
of hydroxyl radicals with sub-micron squalane particles: a model system for
understanding the oxidative aging of ambient aerosols, Atmos. Chem.
Phys., 9, 3209–3222, https://doi.org/10.5194/acp-9-3209-2009, 2009. a
Song, H., Chen, X., Lu, K., Zou, Q., Tan, Z., Fuchs, H., Wiedensohler, A.,
Moon, D. R., Heard, D. E., Baeza-Romero, M.-T., Zheng, M., Wahner, A.,
Kiendler-Scharr, A., and Zhang, Y.: Influence of aerosol copper on
HO2 uptake: a novel parameterized equation, Atmos.
Chem. Phys., 20, 15835–15850, https://doi.org/10.5194/acp-20-15835-2020,
2020. a
Stadtler, S., Simpson, D., Schröder, S., Taraborrelli, D., Bott, A., and Schultz, M.: Ozone impacts of gas–aerosol uptake in global chemistry transport models, Atmos. Chem. Phys., 18, 3147–3171, https://doi.org/10.5194/acp-18-3147-2018, 2018. a
Stohs, S. J. and Bagchi, D.: Oxidative mechanisms in the toxicity of metal
ions, Free Radical Bio. Med., 18, 321–336,
https://doi.org/10.1016/0891-5849(94)00159-h, 1995. a
Takahama, S., Gilardoni, S., and Russell, L. M.: Single-particle oxidation
state and morphology of atmospheric iron aerosols, J. Geophys.
Res.-Atmos., 113, D22202, https://doi.org/10.1029/2008JD009810, 2008. a, b
Taketani, F., Kanaya, Y., and Akimoto, H.: Kinetics of Heterogeneous Reactions
of HO2 Radical at Ambient Concentration Levels with
(NH4)2SO4 and NaCl Aerosol
Particles, J. Phys. Chem. A, 112, 2370–2377,
https://doi.org/10.1021/jp0769936, 2008. a
Taketani, F., Kanaya, Y., Pochanart, P., Liu, Y., Li, J., Okuzawa, K.,
Kawamura, K., Wang, Z., and Akimoto, H.: Measurement of overall uptake
coefficients for HO2 radicals by aerosol particles sampled
from ambient air at Mts. Tai and Mang (China), Atmos. Chem.
Phys., 12, 11907–11916, https://doi.org/10.5194/acp-12-11907-2012, 2012. a
Tan, Z., Hofzumahaus, A., Lu, K., Brown, S. S., Holland, F., Huey, L. G.,
Kiendler-Scharr, A., Li, X., Liu, X., Ma, N., Min, K.-E., Rohrer, F., Shao,
M., Wahner, A., Wang, Y., Wiedensohler, A., Wu, Y., Wu, Z., Zeng, L., Zhang,
Y., and Fuchs, H.: No Evidence for a Significant Impact of Heterogeneous
Chemistry on Radical Concentrations in the North China Plain in Summer 2014,
Environ. Sci. Technol., 54, 5973–5979,
https://doi.org/10.1021/acs.est.0c00525, 2020. a
Thornton, J. and Abbatt, J. P. D.: Measurements of HO2 uptake
to aqueous aerosol: Mass accommodation coefficients and net reactive loss,
J. Geophys. Res., 100, D08309, https://doi.org/10.1029/2004JD005402, 2005. a, b
Tong, H., Arangio, A. M., Lakey, P. S. J., Berkemeier, T., Liu, F., Kampf,
C. J., Brune, W. H., Pöschl, U., and Shiraiwa, M.: Hydroxyl radicals
from secondary organic aerosol decomposition in water, Atmos. Chem. Phys.,
16, 1761–1771, https://doi.org/10.5194/acp-16-1761-2016, 2016. a
Tong, H., Lakey, P. S. J., Arangio, A. M., Socorro, J., Kampf, C. J.,
Berkemeier, T., Brune, W. H., Pöschl, U., and Shiraiwa, M.: Reactive
oxygen species formed in aqueous mixtures of secondary organic aerosols and
mineral dust influencing cloud chemistry and public health in the
Anthropocene, Faraday Discuss., 200, 251–270, https://doi.org/10.1039/C7FD00023E,
2017. a, b, c
Tong, H., Liu, F., Filippi, A., Wilson, J., Arangio, A. M., Zhang, Y., Yue, S., Lelieveld, S., Shen, F., Keskinen, H.-M. K., Li, J., Chen, H., Zhang, T., Hoffmann, T., Fu, P., Brune, W. H., Petäjä, T., Kulmala, M., Yao, M., Berkemeier, T., Shiraiwa, M., and Pöschl, U.: Aqueous-phase reactive species formed by fine particulate matter from remote forests and polluted urban air, Atmos. Chem. Phys., 21, 10439–10455, https://doi.org/10.5194/acp-21-10439-2021, 2021. a
Verma, V., Rico-Martinez, R., Kotra, N., King, L., Liu, J., Snell, T. W., and
Weber, R. J.: Contribution of Water-Soluble and Insoluble Components and
Their Hydrophobic/Hydrophilic Subfractions to the Reactive Oxygen
Species-Generating Potential of Fine Ambient Aerosols, Environ. Sci. Technol., 46, 11384–11392, https://doi.org/10.1021/es302484r, 2012. a
Wang, R., Balkanski, Y., Boucher, O., Bopp, L., Chappell, A., Ciais, P.,
Hauglustaine, D., Peñuelas, J., and Tao, S.: Sources, transport and
deposition of iron in the global atmosphere, Atmos. Chem.
Phys., 15, 6247–6270, https://doi.org/10.5194/acp-15-6247-2015, 2015. a
Waring, C., King, K. L., Bagot, P. A. J., Costen, M. L., and McKendrick, K. G.:
Collision dynamics and reactive uptake of OH radicals at liquid surfaces of
atmospheric interest, Phys. Chem. Chem. Phys., 13, 8457–8469,
https://doi.org/10.1039/C0CP02734K, 2011. a
Wei, J., Fang, T., Wong, C., Lakey, P. S. J., Nizkorodov, S. A., and Shiraiwa,
M.: Superoxide Formation from Aqueous Reactions of Biogenic Secondary
Organic Aerosols, Environ. Sci. Technol., 55, 260–270,
https://doi.org/10.1021/acs.est.0c07789, 2021.
a
Xuan, X., Chen, Z., Gong, Y., Shen, H., and Chen, S.: Partitioning of hydrogen
peroxide in gas-liquid and gas-aerosol phases, Atmos. Chem.
Phys., 20, 5513–5526, https://doi.org/10.5194/acp-20-5513-2020, 2020. a
Zhang, G., Bi, X., Lou, S., Li, L., Wang, H., Wang, X., Zhou, Z., Sheng, G.,
Fu, J., and Chen, C.: Source and mixing state of iron-containing particles
in Shanghai by individual particle analysis, Chemosphere, 95, 9–16,
https://doi.org/10.1016/j.chemosphere.2013.04.046, 2014. a
Zhou, J., Murano, K., Kohno, N., Sakamoto, Y., and Kajii, Y.: Real-time
quantification of the total HO2 reactivity of ambient air and HO2 uptake
kinetics onto ambient aerosols in Kyoto (Japan), Atmos. Environ.,
223, 117189, https://doi.org/10.1016/j.atmosenv.2019.117189, 2020. a
Zhou, J., Sato, K., Bai, Y., Fukusaki, Y., Kousa, Y., Ramasamy, S., Takami, A., Yoshino, A., Nakayama, T., Sadanaga, Y., Nakashima, Y., Li, J., Murano, K., Kohno, N., Sakamoto, Y., and Kajii, Y.: Kinetics and impacting factors of HO2 uptake onto submicron atmospheric aerosols during the 2019 Air QUAlity Study (AQUAS) in Yokohama, Japan , Atmos. Chem. Phys., 21, 12243–12260, https://doi.org/10.5194/acp-21-12243-2021, 2021. a
Short summary
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.
Chemical reactions with iron in clouds and aerosol form and cycle reactive oxygen species (ROS)....
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