Articles | Volume 22, issue 3
https://doi.org/10.5194/acp-22-1989-2022
© Author(s) 2022. 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-22-1989-2022
© Author(s) 2022. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
11 Feb 2022
Research article |
| 11 Feb 2022
| 11 Feb 2022
The number fraction of iron-containing particles affects OH, HO2 and H2O2 budgets in the atmospheric aqueous phase
Amina Khaled
Université Clermont Auvergne, CNRS, SIGMA Clermont, Institut de Chimie de Clermont-Ferrand, 63000 Clermont-Ferrand, France
Minghui Zhang
Université Clermont Auvergne, CNRS, SIGMA Clermont, Institut de Chimie de Clermont-Ferrand, 63000 Clermont-Ferrand, France
now at: Plair SA, Route de Saint-Julien 275, Perly 1258, Switzerland
Université Clermont Auvergne, CNRS, SIGMA Clermont, Institut de Chimie de Clermont-Ferrand, 63000 Clermont-Ferrand, France
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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.
Barbara Ervens, Ken S. Carslaw, Thomas Koop, and Ulrich Pöschl
EGUsphere, https://doi.org/10.5194/egusphere-2025-419, https://doi.org/10.5194/egusphere-2025-419, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Over the past two decades, the European Geosciences Union (EGU) has demonstrated the success, viability and benefits of interactive open access (OA) publishing with public peer review in its journals, its publishing platform EGUsphere and virtual compilations. The article summarizes the evolution of the EGU/Copernicus publications and of OA publishing with interactive public peer review at large by placing the EGU/Copernicus publications in the context of current and future global open science.
Barbara Ervens, Pierre Amato, Kifle Aregahegn, Muriel Joly, Amina Khaled, Tiphaine Labed-Veydert, Frédéric Mathonat, Leslie Nuñez López, Raphaëlle Péguilhan, and Minghui Zhang
Biogeosciences, 22, 243–256, https://doi.org/10.5194/bg-22-243-2025, https://doi.org/10.5194/bg-22-243-2025, 2025
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Atmospheric microorganisms are a small fraction of Earth's microbiome, with bacteria being a significant part. Aerosolized bacteria are airborne for a few days, encountering unique chemical and physical conditions affecting stress levels and survival. We explore chemical and microphysical conditions bacteria encounter, highlighting potential nutrient and oxidant limitations and diverse effects by pollutants, which may ultimately impact the microbiome's role in global ecosystems and biodiversity.
Barbara Ervens, Andrew Rickard, Bernard Aumont, William P. L. Carter, Max McGillen, Abdelwahid Mellouki, John Orlando, Bénédicte Picquet-Varrault, Paul Seakins, William R. Stockwell, Luc Vereecken, and Timothy J. Wallington
Atmos. Chem. Phys., 24, 13317–13339, https://doi.org/10.5194/acp-24-13317-2024, https://doi.org/10.5194/acp-24-13317-2024, 2024
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Chemical mechanisms describe the chemical processes in atmospheric models that are used to describe the changes in the atmospheric composition. Therefore, accurate chemical mechanisms are necessary to predict the evolution of air pollution and climate change. The article describes all steps that are needed to build chemical mechanisms and discusses the advances and needs of experimental and theoretical research activities needed to build reliable chemical mechanisms.
Raphaëlle Péguilhan, Florent Rossi, Muriel Joly, Engy Nasr, Bérénice Batut, François Enault, Barbara Ervens, and Pierre Amato
EGUsphere, https://doi.org/10.5194/egusphere-2024-2338, https://doi.org/10.5194/egusphere-2024-2338, 2024
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Using comparative metagenomics/metatranscriptomics, we examined the functioning of airborne microorganisms in clouds and clear atmosphere; clouds are atmospheric volumes where multiple microbial processes are promoted compared with clear atmosphere; Overrepresented microbial functions of interest include the processing of chemical compounds, biomass production and the regulation of oxidants; - this has implications for biogeochemical cycles and microbial ecology.
Leslie Nuñez López, Pierre Amato, and Barbara Ervens
Atmos. Chem. Phys., 24, 5181–5198, https://doi.org/10.5194/acp-24-5181-2024, https://doi.org/10.5194/acp-24-5181-2024, 2024
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Living bacteria comprise a small particle fraction in the atmosphere. Our model study shows that atmospheric bacteria in clouds may efficiently biodegrade formic and acetic acids that affect the acidity of rain. We conclude that current atmospheric models underestimate losses of these acids as they only consider chemical processes. We suggest that biodegradation can affect atmospheric concentration not only of formic and acetic acids but also of other volatile, moderately soluble organics.
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
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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.
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 and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Impacts of meteorology and emission reductions on haze pollution during the lockdown in the North China Plain
Impact of mineral dust on the global nitrate aerosol direct and indirect radiative effect
The surface tension and cloud condensation nuclei (CCN) activation of sea spray aerosol particles
Exploring the processes controlling secondary inorganic aerosol: evaluating the global GEOS-Chem simulation using a suite of aircraft campaigns
Influence of land cover change on atmospheric organic gases, aerosols, and radiative effects
Quantifying the impacts of marine aerosols over the southeast Atlantic Ocean using a chemical transport model: implications for aerosol–cloud interactions
Quantifying the impact of global nitrate aerosol on tropospheric composition fields and its production from lightning NOx
Driving factors of aerosol acidity: a new hierarchical quantitative analysis framework and its application in Changzhou, China
Understanding the Long-term Trend of Organic Aerosol and the Influences from Anthropogenic Emission and Regional Climate Change in China
Rapid oxidation of phenolic compounds by O3 and HO●: effects of the air–water interface and mineral dust in tropospheric chemical processes
Modeling the contribution of leads to sea spray aerosol in the high Arctic
Impacts of Sea Ice Leads on Sea Salt Aerosols and Atmospheric Chemistry in the Arctic
Importance of aerosol composition and aerosol vertical profiles in global spatial variation in the relationship between PM2.5 and aerosol optical depth
Dimethyl sulfide chemistry over the industrial era: comparison of key oxidation mechanisms and long-term observations
Population exposure to outdoor NO2, black carbon, particle mass, and number concentrations over Paris with multi-scale modelling down to the street scale
The co-benefits of a low-carbon future for PM2.5 and O3 air pollution in Europe
Assessing the effectiveness of SO2, NOx, and NH3 emission reductions in mitigating winter PM2.5 in Taiwan using CMAQ
Modelling of atmospheric concentrations of fungal spores: a 2-year simulation over France using CHIMERE
Cluster-dynamics-based parameterization for sulfuric acid–dimethylamine nucleation: comparison and selection through box and three-dimensional modeling
A Comprehensive Global Modelling Assessment of Nitrate Heterogeneous Formation on Desert Dust
Observed and CMIP6-model-simulated organic aerosol response to drought in the contiguous United States during summertime
Long-term trends in aerosol properties derived from AERONET measurements
Cooling radiative forcing effect enhancement of atmospheric amines and mineral particles caused by heterogeneous uptake and oxidation
Critical Load Exceedances for North America and Europe using an Ensemble of Models and an Investigation of Causes for Environmental Impact Estimate Variability: An AQMEII4 Study
Source-resolved atmospheric metal emissions, concentrations, and deposition fluxes into the East Asian seas
Predicted impacts of heterogeneous chemical pathways on particulate sulfur over Fairbanks, Alaska, the N. Hemisphere, and the Contiguous United States
Analysis of secondary inorganic aerosols over the greater Athens area using the EPISODE–CityChem source dispersion and photochemistry model
Global estimates of ambient reactive nitrogen components during 2000–2100 based on the multi-stage model
The role of naphthalene and its derivatives in the formation of secondary organic aerosol in the Yangtze River Delta region, China
Unveiling the optimal regression model for source apportionment of the oxidative potential of PM10
Investigating the contribution of grown new particles to cloud condensation nuclei with largely varying preexisting particles – Part 2: Modeling chemical drivers and 3-D new particle formation occurrence
Technical note: Influence of different averaging metrics and temporal resolutions on the aerosol pH calculated by thermodynamic modeling
Dual roles of the inorganic aqueous phase on secondary organic aerosol growth from benzene and phenol
Global source apportionment of aerosols into major emission regions and sectors over 1850–2017
Modeling atmospheric brown carbon in the GISS ModelE Earth system model
Observation-constrained kinetic modeling of isoprene SOA formation in the atmosphere
Significant impact of urban tree biogenic emissions on air quality estimated by a bottom-up inventory and chemistry transport modeling
Secondary organic aerosols derived from intermediate-volatility n-alkanes adopt low-viscous phase state
Modeling the drivers of fine PM pollution over Central Europe: impacts and contributions of emissions from different sources
Reaction of SO3 with H2SO4 and its implications for aerosol particle formation in the gas phase and at the air–water interface
Weakened aerosol–radiation interaction exacerbating ozone pollution in eastern China since China's clean air actions
Uncertainties from biomass burning aerosols in air quality models obscure public health impacts in Southeast Asia
Oxidative potential apportionment of atmospheric PM1: a new approach combining high-sensitive online analysers for chemical composition and offline OP measurement technique
Aqueous-phase chemistry of glyoxal with multifunctional reduced nitrogen compounds: a potential missing route for secondary brown carbon
An updated modeling framework to simulate Los Angeles air quality – Part 1: Model development, evaluation, and source apportionment
Frequent haze events associated with transport and stagnation over the corridor between the North China Plain and Yangtze River Delta
Evaluation of WRF-Chem-simulated meteorology and aerosols over northern India during the severe pollution episode of 2016
How well are aerosol–cloud interactions represented in climate models? – Part 1: Understanding the sulfate aerosol production from the 2014–15 Holuhraun eruption
pH regulates the formation of organosulfates and inorganic sulfate from organic peroxide reaction with dissolved SO2 in aquatic media
Technical note: Accurate, reliable, and high-resolution air quality predictions by improving the Copernicus Atmosphere Monitoring Service using a novel statistical post-processing method
Lang Liu, Xin Long, Yi Li, Zengliang Zang, Fengwen Wang, Yan Han, Zhier Bao, Yang Chen, Tian Feng, and Jinxin Yang
Atmos. Chem. Phys., 25, 1569–1585, https://doi.org/10.5194/acp-25-1569-2025, https://doi.org/10.5194/acp-25-1569-2025, 2025
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This study uses WRF-Chem to assess how meteorological conditions and emission reductions affected fine particulate matter (PM2.5) in the North China Plain (NCP). It highlights regional disparities: in the northern NCP, adverse weather negated emission reduction effects. In contrast, the southern NCP featured a PM2.5 decrease due to favorable weather and emission reductions. The research highlighted the interaction between emissions, meteorology, and PM2.5.
Alexandros Milousis, Klaus Klingmüller, Alexandra P. Tsimpidi, Jasper F. Kok, Maria Kanakidou, Athanasios Nenes, and Vlassis A. Karydis
Atmos. Chem. Phys., 25, 1333–1351, https://doi.org/10.5194/acp-25-1333-2025, https://doi.org/10.5194/acp-25-1333-2025, 2025
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This study investigates the impact of dust on the global radiative effect of nitrate aerosols. The results indicate both positive and negative regional shortwave and longwave radiative effects due to aerosol–radiation interactions and cloud adjustments. The global average net REari and REaci of nitrate aerosols are −0.11 and +0.17 W m−2, respectively, mainly affecting the shortwave spectrum. Sensitivity simulations evaluated the influence of mineral dust composition and emissions on the results.
Judith Kleinheins, Nadia Shardt, Ulrike Lohmann, and Claudia Marcolli
Atmos. Chem. Phys., 25, 881–903, https://doi.org/10.5194/acp-25-881-2025, https://doi.org/10.5194/acp-25-881-2025, 2025
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We model the cloud condensation nuclei (CCN) activation of sea spray aerosol particles with classical Köhler theory and with a new model approach that takes surface tension lowering into account. We categorize organic compounds into weak, intermediate, and strong surfactants, and we outline for which composition surface tension lowering is important. The results suggest that surface tension lowering allows sea spray aerosol particles in the Aitken mode to be a source of CCN in marine updraughts.
Olivia G. Norman, Colette L. Heald, Solomon Bililign, Pedro Campuzano-Jost, Hugh Coe, Marc N. Fiddler, Jaime R. Green, Jose L. Jimenez, Katharina Kaiser, Jin Liao, Ann M. Middlebrook, Benjamin A. Nault, John B. Nowak, Johannes Schneider, and André Welti
Atmos. Chem. Phys., 25, 771–795, https://doi.org/10.5194/acp-25-771-2025, https://doi.org/10.5194/acp-25-771-2025, 2025
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This study finds that one component of secondary inorganic aerosols, nitrate, is greatly overestimated by a global atmospheric chemistry model compared to observations from 11 flight campaigns. None of the loss and production pathways explored can explain the nitrate bias alone. The model’s inability to capture the variability in the observations remains and requires future investigation to avoid biases in policy-related studies (i.e., air quality, health, climate impacts of these aerosols).
Ryan Vella, Matthew Forrest, Andrea Pozzer, Alexandra P. Tsimpidi, Thomas Hickler, Jos Lelieveld, and Holger Tost
Atmos. Chem. Phys., 25, 243–262, https://doi.org/10.5194/acp-25-243-2025, https://doi.org/10.5194/acp-25-243-2025, 2025
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This study examines how land cover changes influence biogenic volatile organic compound (BVOC) emissions and atmospheric states. Using a coupled chemistry–climate–vegetation model, we compare present-day land cover (deforested for crops and grazing) with natural vegetation and an extreme reforestation scenario. We find that vegetation changes significantly impact global BVOC emissions and organic aerosols but have a relatively small effect on total aerosols, clouds, and radiative effects.
Mashiat Hossain, Rebecca M. Garland, and Hannah M. Horowitz
Atmos. Chem. Phys., 24, 14123–14143, https://doi.org/10.5194/acp-24-14123-2024, https://doi.org/10.5194/acp-24-14123-2024, 2024
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Our research examines aerosol dynamics over the southeast Atlantic, a region with significant uncertainties in aerosol radiative forcings. Using the GEOS-Chem model, we find that at cloud altitudes, organic aerosols dominate during the biomass burning season, while sulfate aerosols, driven by marine emissions, prevail during peak primary production. These findings highlight the need for accurate representation of marine aerosols in models to improve climate predictions and reduce uncertainties.
Ashok K. Luhar, Anthony C. Jones, and Jonathan M. Wilkinson
Atmos. Chem. Phys., 24, 14005–14028, https://doi.org/10.5194/acp-24-14005-2024, https://doi.org/10.5194/acp-24-14005-2024, 2024
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Nitrate aerosol is often omitted in global chemistry–climate models, partly due to the chemical complexity of its formation process. Using a global model, we show that including nitrate aerosol significantly impacts tropospheric composition fields, such as ozone, and radiation. Additionally, lightning-generated oxides of nitrogen influence both nitrate aerosol mass concentrations and aerosol size distribution, which has important implications for radiative fluxes and indirect aerosol effects.
Xiaolin Duan, Guangjie Zheng, Chuchu Chen, Qiang Zhang, and Kebin He
EGUsphere, https://doi.org/10.5194/egusphere-2024-3584, https://doi.org/10.5194/egusphere-2024-3584, 2024
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Aerosol acidity is an important parameter in atmospheric chemistry, while its driving factors, especially chemical profiles versus meteorological conditions, are not yet fully understood. Here, we established a hierarchical quantitative analysis framework to understand the driving factors of aerosol acidity on different time scales. Its application in Changzhou, China revealed distinct driving factors and corresponding mechanisms of aerosol acidity from annual trends to random residues.
Wenxin Zhang, Yaman Liu, Man Yue, Xinyi Dong, and Minghuai Wang
EGUsphere, https://doi.org/10.5194/egusphere-2024-3420, https://doi.org/10.5194/egusphere-2024-3420, 2024
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Understanding long-term organic aerosols (OA) trends and their driving factors is important for air quality management. Our modeling revealed that OA in China increased by 5.6% from 1990 to 2019, primarily due to a 32.3% increase in secondary organic aerosols (SOA) and an 8.1% decrease in primary organic aerosols (POA), both largely driven by changes in anthropogenic emissions. Biogenic SOA increased due to warming but showed little response to changes in anthropogenic nitrogen oxide emissions.
Yanru Huo, Mingxue Li, Xueyu Wang, Jianfei Sun, Yuxin Zhou, Yuhui Ma, and Maoxia He
Atmos. Chem. Phys., 24, 12409–12423, https://doi.org/10.5194/acp-24-12409-2024, https://doi.org/10.5194/acp-24-12409-2024, 2024
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This work found that the air–water (A–W) interface and TiO2 clusters promote the oxidation of phenolic compounds (PhCs) to varying degrees compared with the gas phase and bulk water. Some byproducts are more harmful than their parent compounds. This work provides important evidence for the rapid oxidation observed in O3/HO• + PhC experiments at the A–W interface and in mineral dust.
Rémy Lapere, Louis Marelle, Pierre Rampal, Laurent Brodeau, Christian Melsheimer, Gunnar Spreen, and Jennie L. Thomas
Atmos. Chem. Phys., 24, 12107–12132, https://doi.org/10.5194/acp-24-12107-2024, https://doi.org/10.5194/acp-24-12107-2024, 2024
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Elongated open-water areas in sea ice, called leads, can release marine aerosols into the atmosphere. In the Arctic, this source of atmospheric particles could play an important role for climate. However, the amount, seasonality and spatial distribution of such emissions are all mostly unknown. Here, we propose a first parameterization for sea spray aerosols emitted through leads in sea ice and quantify their impact on aerosol populations in the high Arctic.
Erin Emme and Hannah Horowitz
EGUsphere, https://doi.org/10.5194/egusphere-2024-3147, https://doi.org/10.5194/egusphere-2024-3147, 2024
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There is uncertainty in the sources of Arctic cold season (November-April) sea salt aerosols. Using a chemical transport model and satellite observations, we quantify Arctic-wide sea salt aerosol emissions from fractures in sea ice, called open sea ice leads, and their atmospheric chemistry impacts for the cold season. We show sea ice leads contribute to Arctic sea salt aerosols and bromine, especially in under-observed regions.
Haihui Zhu, Randall V. Martin, Aaron van Donkelaar, Melanie S. Hammer, Chi Li, Jun Meng, Christopher R. Oxford, Xuan Liu, Yanshun Li, Dandan Zhang, Inderjeet Singh, and Alexei Lyapustin
Atmos. Chem. Phys., 24, 11565–11584, https://doi.org/10.5194/acp-24-11565-2024, https://doi.org/10.5194/acp-24-11565-2024, 2024
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Ambient fine particulate matter (PM2.5) contributes to 4 million deaths globally each year. Satellite remote sensing of aerosol optical depth (AOD), coupled with a simulated PM2.5–AOD relationship (η), can provide global PM2.5 estimations. This study aims to understand the spatial patterns and driving factors of η to guide future measurement and modeling efforts. We quantified η globally and regionally and found that its spatial variation is strongly influenced by aerosol composition.
Ursula A. Jongebloed, Jacob I. Chalif, Linia Tashmim, William C. Porter, Kelvin H. Bates, Qianjie Chen, Erich C. Osterberg, Bess G. Koffman, Jihong Cole-Dai, Dominic A. Winksi, David G. Ferris, Karl J. Kreutz, Cameron P. Wake, and Becky Alexander
EGUsphere, https://doi.org/10.5194/egusphere-2024-3026, https://doi.org/10.5194/egusphere-2024-3026, 2024
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Marine phytoplankton emit dimethyl sulfide (DMS), which forms methanesulfonic acid (MSA) and sulfate. MSA concentrations in ice cores decreased over the industrial era, which has been attributed to pollution-driven changes in DMS chemistry. We use a models to investigate DMS chemistry compared to observations of DMS, MSA, and sulfate. We find that modeled DMS, MSA, and sulfate are influenced by pollution-sensitive oxidant concentrations, characterization of DMS chemistry, and other variables.
Soo-Jin Park, Lya Lugon, Oscar Jacquot, Youngseob Kim, Alexia Baudic, Barbara D’Anna, Ludovico Di Antonio, Claudia Di Biagio, Fabrice Dugay, Olivier Favez, Véronique Ghersi, Aline Gratien, Julien Kammer, Jean-Eudes Petit, Olivier Sanchez, Myrto Valari, Jérémy Vigneron, and Karine Sartelet
EGUsphere, https://doi.org/10.5194/egusphere-2024-2120, https://doi.org/10.5194/egusphere-2024-2120, 2024
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To accurately represent the population exposure to outdoor concentrations of pollutants of health interest (NO2, black carbon, PM2.5, ultrafine particles), multi-scale modelling down to the street scale is setup and evaluated using measurements from field campaigns. An exposure scaling factor is defined, allowing to correct regional-scale simulations to evaluate population exposure. Urban heterogeneities strongly influence NO2, black carbon and ultrafine particles, but less PM2.5.
Connor J. Clayton, Daniel R. Marsh, Steven T. Turnock, Ailish M. Graham, Kirsty J. Pringle, Carly L. Reddington, Rajesh Kumar, and James B. McQuaid
Atmos. Chem. Phys., 24, 10717–10740, https://doi.org/10.5194/acp-24-10717-2024, https://doi.org/10.5194/acp-24-10717-2024, 2024
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We demonstrate that strong climate mitigation could improve air quality in Europe; however, less ambitious mitigation does not result in these co-benefits. We use a high-resolution atmospheric chemistry model. This allows us to demonstrate how this varies across European countries and analyse the underlying chemistry. This may help policy-facing researchers understand which sectors and regions need to be prioritised to achieve strong air quality co-benefits of climate mitigation.
Ping-Chieh Huang, Hui-Ming Hung, Hsin-Chih Lai, and Charles C.-K. Chou
Atmos. Chem. Phys., 24, 10759–10772, https://doi.org/10.5194/acp-24-10759-2024, https://doi.org/10.5194/acp-24-10759-2024, 2024
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Models were used to study ways to reduce particulate matter (PM) pollution in Taiwan during winter. After considering various factors, such as physical processes and chemical reactions, we found that reducing NOx or NH3 emissions is more effective at mitigating PM2.5 than reducing SO2 emissions. When considering both efficiency and cost, reducing NH3 emissions seems to be a more suitable policy for the studied environment in Taiwan.
Matthieu Vida, Gilles Foret, Guillaume Siour, Florian Couvidat, Olivier Favez, Gaelle Uzu, Arineh Cholakian, Sébastien Conil, Matthias Beekmann, and Jean-Luc Jaffrezo
Atmos. Chem. Phys., 24, 10601–10615, https://doi.org/10.5194/acp-24-10601-2024, https://doi.org/10.5194/acp-24-10601-2024, 2024
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We simulate 2 years of atmospheric fungal spores over France and use observations of polyols and primary biogenic factors from positive matrix factorisation. The representation of emissions taking into account a proxy for vegetation surface and specific humidity enables us to reproduce very accurately the seasonal cycle of fungal spores. Furthermore, we estimate that fungal spores can account for 20 % of PM10 and 40 % of the organic fraction of PM10 over vegetated areas in summer.
Jiewen Shen, Bin Zhao, Shuxiao Wang, An Ning, Yuyang Li, Runlong Cai, Da Gao, Biwu Chu, Yang Gao, Manish Shrivastava, Jingkun Jiang, Xiuhui Zhang, and Hong He
Atmos. Chem. Phys., 24, 10261–10278, https://doi.org/10.5194/acp-24-10261-2024, https://doi.org/10.5194/acp-24-10261-2024, 2024
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We extensively compare various cluster-dynamics-based parameterizations for sulfuric acid–dimethylamine nucleation and identify a newly developed parameterization derived from Atmospheric Cluster Dynamic Code (ACDC) simulations as being the most reliable one. This study offers a valuable reference for developing parameterizations of other nucleation systems and is meaningful for the accurate quantification of the environmental and climate impacts of new particle formation.
Rubén Soussé-Villa, Oriol Jorba, María Gonçalves Ageitos, Dene Bowdalo, Marc Guevara, and Carlos Pérez García-Pando
EGUsphere, https://doi.org/10.5194/egusphere-2024-2310, https://doi.org/10.5194/egusphere-2024-2310, 2024
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Desert dust forms nitrate coatings as it travels through the atmosphere. However, current models that predict this process vary greatly due to different methods and inaccuracies. We examined how nitrate forms in a global model, focusing on how gases condense on dust, the lifespan of different particles, and the impact of alkalinity. Our findings show that models work best when they consider reversible gas condensation with alkalinity. This should lead to better estimates of climate impacts.
Wei Li and Yuxuan Wang
Atmos. Chem. Phys., 24, 9339–9353, https://doi.org/10.5194/acp-24-9339-2024, https://doi.org/10.5194/acp-24-9339-2024, 2024
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Droughts immensely increased organic aerosol (OA) in the contiguous United States in summer (1998–2019), notably in the Pacific Northwest (PNW) and Southeast (SEUS). The OA rise in the SEUS is driven by the enhanced formation of epoxydiol-derived secondary organic aerosol due to the increase in biogenic volatile organic compounds and sulfate, while in the PNW, it is caused by wildfires. A total of 10 climate models captured the OA increase in the PNW yet greatly underestimated it in the SEUS.
Zhenyu Zhang, Jing Li, Huizheng Che, Yueming Dong, Oleg Dubovik, Thomas Eck, Pawan Gupta, Brent Holben, Jhoon Kim, Elena Lind, Trailokya Saud, Sachchida Nand Tripathi, and Tong Ying
EGUsphere, https://doi.org/10.5194/egusphere-2024-2533, https://doi.org/10.5194/egusphere-2024-2533, 2024
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We used ground-based remote sensing data from the Aerosol Robotic Network to examine long-term trends in aerosol characteristics. We found aerosol loadings generally decreased globally, and aerosols became more scattering. These changes are closely related to variations in aerosol compositions, such as decreased anthropogenic emissions over East Asia, Europe, and North America, increased anthropogenic source over North India, increased dust activities over the Arabian Peninsula, etc.
Weina Zhang, Jianhua Mai, Zhichao Fan, Yongpeng Ji, Yuemeng Ji, Guiying Li, Yanpeng Gao, and Taicheng An
Atmos. Chem. Phys., 24, 9019–9030, https://doi.org/10.5194/acp-24-9019-2024, https://doi.org/10.5194/acp-24-9019-2024, 2024
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This study reveals heterogeneous oxidation causes further radiative forcing effect (RFE) enhancement of amine–mineral mixed particles. Note that RFE increment is higher under clean conditions than that under polluted conditions, which is contributed to high-oxygen-content products. The enhanced RFE of amine–mineral particles caused by heterogenous oxidation is expected to alleviate warming effects.
Paul A. Makar, Philip Cheung, Christian Hogrefe, Ayodeji Akingunola, Ummugulsum Alyuz-Ozdemir, Jesse O. Bash, Michael D. Bell, Roberto Bellasio, Roberto Bianconi, Tim Butler, Hazel Cathcart, Olivia E. Clifton, Alma Hodzic, Iannis Koutsioukis, Richard Kranenburg, Aurelia Lupascu, Jason A. Lynch, Kester Momoh, Juan L. Perez-Camanyo, Jonathan Pleim, Young-Hee Ryu, Roberto San Jose, Donna Schwede, Thomas Scheuschner, Mark Shephard, Ranjeet Sokhi, and Stefano Galmarini
EGUsphere, https://doi.org/10.5194/egusphere-2024-2226, https://doi.org/10.5194/egusphere-2024-2226, 2024
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The large range of sulphur and nitrogen deposition estimates from air-quality models results in a large range of predicted impacts. We used models and deposition diagnostics to identify the processes controlling atmospheric sulphur and nitrogen deposition variability. Controlling factors included the uptake of gases and aerosols by droplets, rain, snow, etc., aerosol inorganic chemistry, particle dry deposition, ammonia bidirectional fluxes, and gas deposition via plant cuticles and soil.
Shenglan Jiang, Yan Zhang, Guangyuan Yu, Zimin Han, Junri Zhao, Tianle Zhang, and Mei Zheng
Atmos. Chem. Phys., 24, 8363–8381, https://doi.org/10.5194/acp-24-8363-2024, https://doi.org/10.5194/acp-24-8363-2024, 2024
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This study aims to provide gridded data on sea-wide concentrations, deposition fluxes, and soluble deposition fluxes with detailed source categories of metals using the modified CMAQ model. We developed a monthly emission inventory of six metals – Fe, Al, V, Ni, Zn, and Cu – from terrestrial anthropogenic, ship, and dust sources in East Asia in 2017. Our results reveal the contribution of each source to the emissions, concentrations, and deposition fluxes of metals in the East Asian seas.
Sara Louise Farrell, Havala O. T. Pye, Robert Gilliam, George Pouliot, Deanna Huff, Golam Sarwar, William Vizuete, Nicole Briggs, and Kathleen Fahey
EGUsphere, https://doi.org/10.5194/egusphere-2024-1550, https://doi.org/10.5194/egusphere-2024-1550, 2024
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In this work we implement heterogeneous sulfur chemistry into the Community Multiscale Air Quality (CMAQ) model. This new chemistry accounts for the formation of sulfate via aqueous oxidation of SO2 in aerosol liquid water and the formation of hydroxymethanesulfonate (HMS) – often confused by measurement techniques as sulfate. Model performance in predicting sulfur PM2.5 in Fairbanks, Alaska, and other places that experience dark and cold winters, is improved.
Stelios Myriokefalitakis, Matthias Karl, Kim A. Weiss, Dimitris Karagiannis, Eleni Athanasopoulou, Anastasia Kakouri, Aikaterini Bougiatioti, Eleni Liakakou, Iasonas Stavroulas, Georgios Papangelis, Georgios Grivas, Despina Paraskevopoulou, Orestis Speyer, Nikolaos Mihalopoulos, and Evangelos Gerasopoulos
Atmos. Chem. Phys., 24, 7815–7835, https://doi.org/10.5194/acp-24-7815-2024, https://doi.org/10.5194/acp-24-7815-2024, 2024
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A state-of-the-art thermodynamic model has been coupled with the city-scale chemistry transport model EPISODE–CityChem to investigate the equilibrium between the inorganic gas and aerosol phases over the greater Athens area, Greece. The simulations indicate that the formation of nitrates in an urban environment is significantly affected by local nitrogen oxide emissions, as well as ambient temperature, relative humidity, photochemical activity, and the presence of non-volatile cations.
Rui Li, Yining Gao, Lijia Zhang, Yubing Shen, Tianzhao Xu, Wenwen Sun, and Gehui Wang
Atmos. Chem. Phys., 24, 7623–7636, https://doi.org/10.5194/acp-24-7623-2024, https://doi.org/10.5194/acp-24-7623-2024, 2024
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A three-stage model was developed to obtain the global maps of reactive nitrogen components during 2000–2100. The results implied that cross-validation R2 values of four species showed satisfactory performance (R2 > 0.55). Most reactive nitrogen components, except NH3, in China showed increases during 2000–2013. In the future scenarios, SSP3-7.0 (traditional-energy scenario) and SSP1-2.6 (carbon neutrality scenario) showed the highest and lowest reactive nitrogen component concentrations.
Fei Ye, Jingyi Li, Yaqin Gao, Hongli Wang, Jingyu An, Cheng Huang, Song Guo, Keding Lu, Kangjia Gong, Haowen Zhang, Momei Qin, and Jianlin Hu
Atmos. Chem. Phys., 24, 7467–7479, https://doi.org/10.5194/acp-24-7467-2024, https://doi.org/10.5194/acp-24-7467-2024, 2024
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Naphthalene (Nap) and methylnaphthalene (MN) are key precursors of secondary organic aerosol (SOA), yet their sources and sinks are often inadequately represented in air quality models. In this study, we incorporated detailed emissions, gas-phase chemistry, and SOA parameterization of Nap and MN into CMAQ to address this issue. The findings revealed remarkably high SOA formation potentials for these compounds despite their low emissions in the Yangtze River Delta region during summer.
Vy Dinh Ngoc Thuy, Jean-Luc Jaffrezo, Ian Hough, Pamela A. Dominutti, Guillaume Salque Moreton, Grégory Gille, Florie Francony, Arabelle Patron-Anquez, Olivier Favez, and Gaëlle Uzu
Atmos. Chem. Phys., 24, 7261–7282, https://doi.org/10.5194/acp-24-7261-2024, https://doi.org/10.5194/acp-24-7261-2024, 2024
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The capacity of particulate matter (PM) to generate reactive oxygen species in vivo is represented by oxidative potential (OP). This study focuses on finding the appropriate model to evaluate the oxidative character of PM sources in six sites using the PM sources and OP. Eight regression techniques are introduced to assess the OP of PM. The study highlights the importance of selecting a model according to the input data characteristics and establishes some recommendations for the procedure.
Ming Chu, Xing Wei, Shangfei Hai, Yang Gao, Huiwang Gao, Yujiao Zhu, Biwu Chu, Nan Ma, Juan Hong, Yele Sun, and Xiaohong Yao
Atmos. Chem. Phys., 24, 6769–6786, https://doi.org/10.5194/acp-24-6769-2024, https://doi.org/10.5194/acp-24-6769-2024, 2024
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We used a 20-bin WRF-Chem model to simulate NPF events in the NCP during a three-week observational period in the summer of 2019. The model was able to reproduce the observations during June 29–July 6, which was characterized by a high frequency of NPF occurrence.
Haoqi Wang, Xiao Tian, Wanting Zhao, Jiacheng Li, Haoyu Yu, Yinchang Feng, and Shaojie Song
Atmos. Chem. Phys., 24, 6583–6592, https://doi.org/10.5194/acp-24-6583-2024, https://doi.org/10.5194/acp-24-6583-2024, 2024
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pH is a key property of ambient aerosols, which affect many atmospheric processes. As aerosol pH is a non-conservative parameter, diverse averaging metrics and temporal resolutions may influence the pH values calculated by thermodynamic models. This technical note seeks to quantitatively evaluate the average pH using varied metrics and resolutions. The ultimate goal is to establish standardized reporting practices in future research endeavors.
Jiwon Choi, Myoseon Jang, and Spencer Blau
Atmos. Chem. Phys., 24, 6567–6582, https://doi.org/10.5194/acp-24-6567-2024, https://doi.org/10.5194/acp-24-6567-2024, 2024
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Persistent phenoxy radical (PPR), formed by phenol gas oxidation and its aqueous reaction, catalytically destroys O3 and retards secondary organic aerosol (SOA) growth. Explicit gas mechanisms including the formation of PPR and low-volatility products from the oxidation of phenol or benzene are applied to the UNIPAR model to predict SOA mass via multiphase reactions of precursors. Aqueous reactions of reactive organics increase SOA mass but retard SOA growth via heterogeneously formed PPR.
Yang Yang, Shaoxuan Mou, Hailong Wang, Pinya Wang, Baojie Li, and Hong Liao
Atmos. Chem. Phys., 24, 6509–6523, https://doi.org/10.5194/acp-24-6509-2024, https://doi.org/10.5194/acp-24-6509-2024, 2024
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The variations in anthropogenic aerosol concentrations and source contributions and their subsequent radiative impact in major emission regions during historical periods are quantified based on an aerosol-tagging system in E3SMv1. Due to the industrial development and implementation of economic policies, sources of anthropogenic aerosols show different variations, which has important implications for pollution prevention and control measures and decision-making for global collaboration.
Maegan A. DeLessio, Kostas Tsigaridis, Susanne E. Bauer, Jacek Chowdhary, and Gregory L. Schuster
Atmos. Chem. Phys., 24, 6275–6304, https://doi.org/10.5194/acp-24-6275-2024, https://doi.org/10.5194/acp-24-6275-2024, 2024
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This study presents the first explicit representation of brown carbon aerosols in the GISS ModelE Earth system model (ESM). Model sensitivity to a range of brown carbon parameters and model performance compared to AERONET and MODIS retrievals of total aerosol properties were assessed. A summary of best practices for incorporating brown carbon into ModelE is also included.
Chuanyang Shen, Xiaoyan Yang, Joel Thornton, John Shilling, Chenyang Bi, Gabriel Isaacman-VanWertz, and Haofei Zhang
Atmos. Chem. Phys., 24, 6153–6175, https://doi.org/10.5194/acp-24-6153-2024, https://doi.org/10.5194/acp-24-6153-2024, 2024
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In this work, a condensed multiphase isoprene oxidation mechanism was developed to simulate isoprene SOA formation from chamber and field studies. Our results show that the measured isoprene SOA mass concentrations can be reasonably reproduced. The simulation results indicate that multifunctional low-volatility products contribute significantly to total isoprene SOA. Our findings emphasize that the pathways to produce these low-volatility species should be considered in models.
Alice Maison, Lya Lugon, Soo-Jin Park, Alexia Baudic, Christopher Cantrell, Florian Couvidat, Barbara D'Anna, Claudia Di Biagio, Aline Gratien, Valérie Gros, Carmen Kalalian, Julien Kammer, Vincent Michoud, Jean-Eudes Petit, Marwa Shahin, Leila Simon, Myrto Valari, Jérémy Vigneron, Andrée Tuzet, and Karine Sartelet
Atmos. Chem. Phys., 24, 6011–6046, https://doi.org/10.5194/acp-24-6011-2024, https://doi.org/10.5194/acp-24-6011-2024, 2024
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This study presents the development of a bottom-up inventory of urban tree biogenic emissions. Emissions are computed for each tree based on their location and characteristics and are integrated in the regional air quality model WRF-CHIMERE. The impact of these biogenic emissions on air quality is quantified for June–July 2022. Over Paris city, urban trees increase the concentrations of particulate organic matter by 4.6 %, of PM2.5 by 0.6 %, and of ozone by 1.0 % on average over 2 months.
Tommaso Galeazzo, Bernard Aumont, Marie Camredon, Richard Valorso, Yong B. Lim, Paul J. Ziemann, and Manabu Shiraiwa
Atmos. Chem. Phys., 24, 5549–5565, https://doi.org/10.5194/acp-24-5549-2024, https://doi.org/10.5194/acp-24-5549-2024, 2024
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Secondary organic aerosol (SOA) derived from n-alkanes is a major component of anthropogenic particulate matter. We provide an analysis of n-alkane SOA by chemistry modeling, machine learning, and laboratory experiments, showing that n-alkane SOA adopts low-viscous semi-solid or liquid states. Our results indicate few kinetic limitations of mass accommodation in SOA formation, supporting the application of equilibrium partitioning for simulating n-alkane SOA in large-scale atmospheric models.
Lukáš Bartík, Peter Huszár, Jan Karlický, Ondřej Vlček, and Kryštof Eben
Atmos. Chem. Phys., 24, 4347–4387, https://doi.org/10.5194/acp-24-4347-2024, https://doi.org/10.5194/acp-24-4347-2024, 2024
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The presented study deals with the attribution of fine particulate matter (PM2.5) concentrations to anthropogenic emissions over Central Europe using regional-scale models. It calculates the present-day contributions of different emissions sectors to concentrations of PM2.5 and its secondary components. Moreover, the study investigates the effect of chemical nonlinearities by using multiple source attribution methods and secondary organic aerosol calculation methods.
Rui Wang, Yang Cheng, Shasha Chen, Rongrong Li, Yue Hu, Xiaokai Guo, Tianlei Zhang, Fengmin Song, and Hao Li
Atmos. Chem. Phys., 24, 4029–4046, https://doi.org/10.5194/acp-24-4029-2024, https://doi.org/10.5194/acp-24-4029-2024, 2024
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We used quantum chemical calculations, Born–Oppenheimer molecular dynamics simulations, and the ACDC kinetic model to characterize SO3–H2SO4 interaction in the gas phase and at the air–water interface and to study the effect of H2S2O7 on H2SO4–NH3-based clusters. The work expands our understanding of new pathways for the loss of SO3 in acidic polluted areas and helps reveal some missing sources of NPF in metropolitan industrial regions and understand the atmospheric organic–sulfur cycle better.
Hao Yang, Lei Chen, Hong Liao, Jia Zhu, Wenjie Wang, and Xin Li
Atmos. Chem. Phys., 24, 4001–4015, https://doi.org/10.5194/acp-24-4001-2024, https://doi.org/10.5194/acp-24-4001-2024, 2024
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The present study quantifies the response of aerosol–radiation interaction (ARI) to anthropogenic emission reduction from 2013 to 2017, with the main focus on the contribution to changed O3 concentrations over eastern China both in summer and winter using the WRF-Chem model. The weakened ARI due to decreased anthropogenic emission aggravates the summer (winter) O3 pollution by +0.81 ppb (+0.63 ppb), averaged over eastern China.
Margaret R. Marvin, Paul I. Palmer, Fei Yao, Mohd Talib Latif, and Md Firoz Khan
Atmos. Chem. Phys., 24, 3699–3715, https://doi.org/10.5194/acp-24-3699-2024, https://doi.org/10.5194/acp-24-3699-2024, 2024
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We use an atmospheric chemistry model to investigate aerosols emitted from fire activity across Southeast Asia. We find that the limited nature of measurements in this region leads to large uncertainties that significantly hinder the model representation of these aerosols and their impacts on air quality. As a result, the number of monthly attributable deaths is underestimated by as many as 4500, particularly in March at the peak of the mainland burning season.
Julie Camman, Benjamin Chazeau, Nicolas Marchand, Amandine Durand, Grégory Gille, Ludovic Lanzi, Jean-Luc Jaffrezo, Henri Wortham, and Gaëlle Uzu
Atmos. Chem. Phys., 24, 3257–3278, https://doi.org/10.5194/acp-24-3257-2024, https://doi.org/10.5194/acp-24-3257-2024, 2024
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Fine particle (PM1) pollution is a major health issue in the city of Marseille, which is subject to numerous pollution sources. Sampling carried out during the summer enabled a fine characterization of the PM1 sources and their oxidative potential, a promising new metric as a proxy for health impact. PM1 came mainly from combustion sources, secondary ammonium sulfate, and organic nitrate, while the oxidative potential of PM1 came from these sources and from resuspended dust in the atmosphere.
Yuemeng Ji, Zhang Shi, Wenjian Li, Jiaxin Wang, Qiuju Shi, Yixin Li, Lei Gao, Ruize Ma, Weijun Lu, Lulu Xu, Yanpeng Gao, Guiying Li, and Taicheng An
Atmos. Chem. Phys., 24, 3079–3091, https://doi.org/10.5194/acp-24-3079-2024, https://doi.org/10.5194/acp-24-3079-2024, 2024
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The formation mechanisms for secondary brown carbon (SBrC) contributed by multifunctional reduced nitrogen compounds (RNCs) remain unclear. Hence, from combined laboratory experiments and quantum chemical calculations, we investigated the heterogeneous reactions of glyoxal (GL) with multifunctional RNCs, which are driven by four-step indirect nucleophilic addition reactions. Our results show a possible missing source for SBrC formation on urban, regional, and global scales.
Elyse A. Pennington, Yuan Wang, Benjamin C. Schulze, Karl M. Seltzer, Jiani Yang, Bin Zhao, Zhe Jiang, Hongru Shi, Melissa Venecek, Daniel Chau, Benjamin N. Murphy, Christopher M. Kenseth, Ryan X. Ward, Havala O. T. Pye, and John H. Seinfeld
Atmos. Chem. Phys., 24, 2345–2363, https://doi.org/10.5194/acp-24-2345-2024, https://doi.org/10.5194/acp-24-2345-2024, 2024
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To assess the air quality in Los Angeles (LA), we improved the CMAQ model by using dynamic traffic emissions and new secondary organic aerosol schemes to represent volatile chemical products. Source apportionment demonstrates that the urban areas of the LA Basin and vicinity are NOx-saturated, with the largest sensitivity of O3 to changes in volatile organic compounds in the urban core. The improvement and remaining issues shed light on the future direction of the model development.
Feifan Yan, Hang Su, Yafang Cheng, Rujin Huang, Hong Liao, Ting Yang, Yuanyuan Zhu, Shaoqing Zhang, Lifang Sheng, Wenbin Kou, Xinran Zeng, Shengnan Xiang, Xiaohong Yao, Huiwang Gao, and Yang Gao
Atmos. Chem. Phys., 24, 2365–2376, https://doi.org/10.5194/acp-24-2365-2024, https://doi.org/10.5194/acp-24-2365-2024, 2024
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PM2.5 pollution is a major air quality issue deteriorating human health, and previous studies mostly focus on regions like the North China Plain and Yangtze River Delta. However, the characteristics of PM2.5 concentrations between these two regions are studied less often. Focusing on the transport corridor region, we identify an interesting seesaw transport phenomenon with stagnant weather conditions, conducive to PM2.5 accumulation over this region, resulting in large health effects.
Prerita Agarwal, David S. Stevenson, and Mathew R. Heal
Atmos. Chem. Phys., 24, 2239–2266, https://doi.org/10.5194/acp-24-2239-2024, https://doi.org/10.5194/acp-24-2239-2024, 2024
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Air pollution levels across northern India are amongst some of the worst in the world, with episodic and hazardous haze events. Here, the ability of the WRF-Chem model to predict air quality over northern India is assessed against several datasets. Whilst surface wind speed and particle pollution peaks are over- and underestimated, respectively, meteorology and aerosol trends are adequately captured, and we conclude it is suitable for investigating severe particle pollution events.
George Jordan, Florent Malavelle, Ying Chen, Amy Peace, Eliza Duncan, Daniel G. Partridge, Paul Kim, Duncan Watson-Parris, Toshihiko Takemura, David Neubauer, Gunnar Myhre, Ragnhild Skeie, Anton Laakso, and James Haywood
Atmos. Chem. Phys., 24, 1939–1960, https://doi.org/10.5194/acp-24-1939-2024, https://doi.org/10.5194/acp-24-1939-2024, 2024
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The 2014–15 Holuhraun eruption caused a huge aerosol plume in an otherwise unpolluted region, providing a chance to study how aerosol alters cloud properties. This two-part study uses observations and models to quantify this relationship’s impact on the Earth’s energy budget. Part 1 suggests the models capture the observed spatial and chemical evolution of the plume, yet no model plume is exact. Understanding these differences is key for Part 2, where changes to cloud properties are explored.
Lin Du, Xiaofan Lv, Makroni Lily, Kun Li, and Narcisse Tsona Tchinda
Atmos. Chem. Phys., 24, 1841–1853, https://doi.org/10.5194/acp-24-1841-2024, https://doi.org/10.5194/acp-24-1841-2024, 2024
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This study explores the pH effect on the reaction of dissolved SO2 with selected organic peroxides. Results show that the formation of organic and/or inorganic sulfate from these peroxides strongly depends on their electronic structures, and these processes are likely to alter the chemical composition of dissolved organic matter in different ways. The rate constants of these reactions exhibit positive pH and temperature dependencies within pH 1–10 and 240–340 K ranges.
Angelo Riccio and Elena Chianese
Atmos. Chem. Phys., 24, 1673–1689, https://doi.org/10.5194/acp-24-1673-2024, https://doi.org/10.5194/acp-24-1673-2024, 2024
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Starting from the Copernicus Atmosphere Monitoring Service (CAMS), we provided a novel ensemble statistical post-processing approach to improve their air quality predictions. Our approach is able to provide reliable short-term forecasts of pollutant concentrations, which is a key challenge in supporting national authorities in their tasks related to EU Air Quality Directives, such as planning and reporting the state of air quality to the citizens.
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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