Articles | Volume 15, issue 16
https://doi.org/10.5194/acp-15-9109-2015
© Author(s) 2015. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-15-9109-2015
© Author(s) 2015. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
17 Aug 2015
Research article |
| 17 Aug 2015
Aqueous-phase oligomerization of methyl vinyl ketone through photooxidation – Part 2: Development of the chemical mechanism and atmospheric implications
Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, Colorado, USA
Chemical Sciences Division, NOAA Earth System Research Laboratory, Boulder, Colorado, USA
P. Renard
Aix Marseille Université, CNRS, LCE FRE 3416, 13331, Marseille, France
S. Tlili
Aix Marseille Université, CNRS, LCE FRE 3416, 13331, Marseille, France
S. Ravier
Aix Marseille Université, CNRS, LCE FRE 3416, 13331, Marseille, France
J.-L. Clément
Aix Marseille Université, CNRS, ICR UMR7273, 13397, Marseille, France
A. Monod
Aix Marseille Université, CNRS, LCE FRE 3416, 13331, Marseille, France
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By performing source-apportionment modeling, the amount of primary and secondary organic emissions was resolved from a bulk aerosol data set measured adjacent to a major highway in France. Over 70% of vehicles on this highway were diesel, and a high concentration of BC and NOx were measured. Even close to a major highway, the bulk of the aerosol mass was secondary in nature. Radiocarbon data revealed that most of the fossil organic carbon was from primary vehicular emissions and not from SOA.
C. Denjean, P. Formenti, B. Picquet-Varrault, E. Pangui, P. Zapf, Y. Katrib, C. Giorio, A. Tapparo, A. Monod, B. Temime-Roussel, P. Decorse, C. Mangeney, and J. F. Doussin
Atmos. Chem. Phys., 15, 3339–3358, https://doi.org/10.5194/acp-15-3339-2015, https://doi.org/10.5194/acp-15-3339-2015, 2015
L. Brégonzio-Rozier, F. Siekmann, C. Giorio, E. Pangui, S. B. Morales, B. Temime-Roussel, A. Gratien, V. Michoud, S. Ravier, M. Cazaunau, A. Tapparo, A. Monod, and J.-F. Doussin
Atmos. Chem. Phys., 15, 2953–2968, https://doi.org/10.5194/acp-15-2953-2015, https://doi.org/10.5194/acp-15-2953-2015, 2015
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First- and higher order -generation products formed from the oxidation of isoprene and methacrolein with OH radicals in the presence of NOx have been studied in a simulation chamber. Differences in light source are proposed to partially explain the discrepancies observed between different studies in the literature for both isoprene- and methacrolein-SOA mass yields. According to our results, these SOA yields in the atmosphere could be lower than suggested by most of the current chamber studies.
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.
C. Denjean, P. Formenti, B. Picquet-Varrault, M. Camredon, E. Pangui, P. Zapf, Y. Katrib, C. Giorio, A. Tapparo, B. Temime-Roussel, A. Monod, B. Aumont, and J. F. Doussin
Atmos. Chem. Phys., 15, 883–897, https://doi.org/10.5194/acp-15-883-2015, https://doi.org/10.5194/acp-15-883-2015, 2015
P. Renard, F. Siekmann, G. Salque, C. Demelas, B. Coulomb, L. Vassalo, S. Ravier, B. Temime-Roussel, D. Voisin, and A. Monod
Atmos. Chem. Phys., 15, 21–35, https://doi.org/10.5194/acp-15-21-2015, https://doi.org/10.5194/acp-15-21-2015, 2015
J.-F. Doussin and A. Monod
Atmos. Chem. Phys., 13, 11625–11641, https://doi.org/10.5194/acp-13-11625-2013, https://doi.org/10.5194/acp-13-11625-2013, 2013
P. Renard, F. Siekmann, A. Gandolfo, J. Socorro, G. Salque, S. Ravier, E. Quivet, J.-L. Clément, M. Traikia, A.-M. Delort, D. Voisin, V. Vuitton, R. Thissen, and A. Monod
Atmos. Chem. Phys., 13, 6473–6491, https://doi.org/10.5194/acp-13-6473-2013, https://doi.org/10.5194/acp-13-6473-2013, 2013
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)
Modeling the contribution of leads to sea spray aerosol in the high Arctic
Importance of aerosol composition and aerosol vertical profiles in global spatial variation in the relationship between PM2.5 and aerosol optical depth
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
Observed and CMIP6-model-simulated organic aerosol response to drought in the contiguous United States during summertime
Cooling radiative forcing effect enhancement of atmospheric amines and mineral particles caused by heterogeneous uptake and oxidation
Source-resolved atmospheric metal emissions, concentrations, and deposition fluxes into the East Asian seas
Quantifying the impact of global nitrate aerosol on tropospheric composition fields and its production from lightning NOx
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
Quantifying the Impacts of Marine Aerosols over the Southeast Atlantic Ocean using a chemical transport model: Implications for aerosol-cloud interactions
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
Measurement report: Rapid oxidation of phenolic compounds by O3 and HO•: effects of air-water interface and mineral dust in tropospheric chemical processes
Contribution of intermediate-volatility organic compounds from on-road transport to secondary organic aerosol levels in Europe
Development of an integrated model framework for multi-air-pollutant exposure assessments in high-density cities
CAMx–UNIPAR simulation of secondary organic aerosol mass formed from multiphase reactions of hydrocarbons under the Central Valley urban atmospheres of California
Impact of urbanization on fine particulate matter concentrations over central Europe
Measurement report: Assessing the impacts of emission uncertainty on aerosol optical properties and radiative forcing from biomass burning in peninsular Southeast Asia
The Emissions Model Intercomparison Project (Emissions-MIP): quantifying model sensitivity to emission characteristics
Dynamics-based estimates of decline trend with fine temporal variations in China's PM2.5 emissions
Effects of simulated secondary organic aerosol water on PM1 levels and composition over the US
Reactive organic carbon air emissions from mobile sources in the United States
Development and evaluation of processes affecting simulation of diel fine particulate matter variation in the GEOS-Chem model
Substantially positive contributions of new particle formation to cloud condensation nuclei under low supersaturation in China based on numerical model improvements
Evolution of atmospheric age of particles and its implications for the formation of a severe haze event in eastern China
A multimodel evaluation of the potential impact of shipping on particle species in the Mediterranean Sea
How does tropospheric VOC chemistry affect climate? An investigation of preindustrial control simulations using the Community Earth System Model version 2
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.
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.
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.
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.
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.
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.
Ashok K. Luhar, Anthony C. Jones, and Jonathan M. Wilkinson
EGUsphere, https://doi.org/10.5194/egusphere-2024-1363, https://doi.org/10.5194/egusphere-2024-1363, 2024
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Nitrate aerosol is often omitted in global chemistry-climate models due to the chemical complexity of its formation process. Using a global model, we demonstrate 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.
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.
Mashiat Hossain, Rebecca M. Garland, and Hannah M. Horowitz
EGUsphere, https://doi.org/10.5194/egusphere-2024-1948, https://doi.org/10.5194/egusphere-2024-1948, 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.
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.
Yanru Huo, Mingxue Li, Xueyu Wang, Jianfei Sun, Yuxin Zhou, Yuhui Ma, and Maoxia He
EGUsphere, https://doi.org/10.5194/egusphere-2023-2856, https://doi.org/10.5194/egusphere-2023-2856, 2024
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This work found that the A-W interface and TiO2 clusters promote the oxidation of phenolic compounds (PhCs) to varying degrees comparing with gas phase, and bulk water. Some by-products are more harmful than their parent compounds. This work provides important evidence for the rapid oxidation observed in the O3/HO• + PhCs experiments at the A-W interface and in the mineral dust.
Stella E. I. Manavi and Spyros N. Pandis
Atmos. Chem. Phys., 24, 891–909, https://doi.org/10.5194/acp-24-891-2024, https://doi.org/10.5194/acp-24-891-2024, 2024
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Organic vapors of intermediate volatility have often been neglected as sources of atmospheric organic aerosol. In this work we use a new approach for their simulation and quantify the contribution of these compounds emitted by transportation sources (gasoline and diesel vehicles) to particulate matter over Europe. The estimated secondary organic aerosol levels are on average 60 % higher than predicted by previous approaches. However, these estimates are probably lower limits.
Zhiyuan Li, Kin-Fai Ho, Harry Fung Lee, and Steve Hung Lam Yim
Atmos. Chem. Phys., 24, 649–661, https://doi.org/10.5194/acp-24-649-2024, https://doi.org/10.5194/acp-24-649-2024, 2024
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This study developed an integrated model framework for accurate multi-air-pollutant exposure assessments in high-density and high-rise cities. Following the proposed integrated model framework, we established multi-air-pollutant exposure models for four major PM10 chemical species as well as four criteria air pollutants with R2 values ranging from 0.73 to 0.93. The proposed framework serves as an important tool for combined exposure assessment in epidemiological studies.
Yujin Jo, Myoseon Jang, Sanghee Han, Azad Madhu, Bonyoung Koo, Yiqin Jia, Zechen Yu, Soontae Kim, and Jinsoo Park
Atmos. Chem. Phys., 24, 487–508, https://doi.org/10.5194/acp-24-487-2024, https://doi.org/10.5194/acp-24-487-2024, 2024
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The CAMx–UNIPAR model simulated the SOA budget formed via multiphase reactions of hydrocarbons and the impact of emissions and climate on SOA characteristics under California’s urban environments during winter 2018. SOA growth was dominated by daytime oxidation of long-chain alkanes and nighttime terpene oxidation with O3 and NO−3 radicals. The spatial distributions of anthropogenic SOA were affected by the northwesterly wind, whereas those of biogenic SOA were insensitive to wind directions.
Peter Huszar, Alvaro Patricio Prieto Perez, Lukáš Bartík, Jan Karlický, and Anahi Villalba-Pradas
Atmos. Chem. Phys., 24, 397–425, https://doi.org/10.5194/acp-24-397-2024, https://doi.org/10.5194/acp-24-397-2024, 2024
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Urbanization transforms rural land into artificial land, while due to human activities, it also introduces a great quantity of emissions. We quantify the impact of urbanization on the final particulate matter pollutant levels by looking not only at these emissions, but also at the way urban land cover influences meteorological conditions, how the removal of pollutants changes due to urban land cover, and how biogenic emissions from vegetation change due to less vegetation in urban areas.
Yinbao Jin, Yiming Liu, Xiao Lu, Xiaoyang Chen, Ao Shen, Haofan Wang, Yinping Cui, Yifei Xu, Siting Li, Jian Liu, Ming Zhang, Yingying Ma, and Qi Fan
Atmos. Chem. Phys., 24, 367–395, https://doi.org/10.5194/acp-24-367-2024, https://doi.org/10.5194/acp-24-367-2024, 2024
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This study aims to address these issues by evaluating eight independent biomass burning (BB) emission inventories (GFED, FINN1.5, FINN2.5 MOS, FINN2.5 MOSVIS, GFAS, FEER, QFED, and IS4FIRES) using the WRF-Chem model and analyzing their impact on aerosol optical properties (AOPs) and direct radiative forcing (DRF) during wildfire events in peninsular Southeast Asia (PSEA) that occurred in March 2019.
Hamza Ahsan, Hailong Wang, Jingbo Wu, Mingxuan Wu, Steven J. Smith, Susanne Bauer, Harrison Suchyta, Dirk Olivié, Gunnar Myhre, Hitoshi Matsui, Huisheng Bian, Jean-François Lamarque, Ken Carslaw, Larry Horowitz, Leighton Regayre, Mian Chin, Michael Schulz, Ragnhild Bieltvedt Skeie, Toshihiko Takemura, and Vaishali Naik
Atmos. Chem. Phys., 23, 14779–14799, https://doi.org/10.5194/acp-23-14779-2023, https://doi.org/10.5194/acp-23-14779-2023, 2023
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We examine the impact of the assumed effective height of SO2 injection, SO2 and BC emission seasonality, and the assumed fraction of SO2 emissions injected as SO4 on climate and chemistry model results. We find that the SO2 injection height has a large impact on surface SO2 concentrations and, in some models, radiative flux. These assumptions are a
hiddensource of inter-model variability and may be leading to bias in some climate model results.
Zhen Peng, Lili Lei, Zhe-Min Tan, Meigen Zhang, Aijun Ding, and Xingxia Kou
Atmos. Chem. Phys., 23, 14505–14520, https://doi.org/10.5194/acp-23-14505-2023, https://doi.org/10.5194/acp-23-14505-2023, 2023
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Annual PM2.5 emissions in China consistently decreased by about 3% to 5% from 2017 to 2020 with spatial variations and seasonal dependencies. High-temporal-resolution and dynamics-based PM2.5 emission estimates provide quantitative diurnal variations for each season. Significant reductions in PM2.5 emissions in the North China Plain and northeast of China in 2020 were caused by COVID-19.
Stylianos Kakavas, Spyros N. Pandis, and Athanasios Nenes
Atmos. Chem. Phys., 23, 13555–13564, https://doi.org/10.5194/acp-23-13555-2023, https://doi.org/10.5194/acp-23-13555-2023, 2023
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Water uptake from organic species in aerosol can affect the partitioning of semi-volatile inorganic compounds but are not considered in global and chemical transport models. We address this with a version of the PM-CAMx model that considers such organic water effects and use it to carry out 1-year aerosol simulations over the continental US. We show that such organic water impacts can increase dry PM1 levels by up to 2 μg m-3 when RH levels and PM1 concentrations are high.
Benjamin N. Murphy, Darrell Sonntag, Karl M. Seltzer, Havala O. T. Pye, Christine Allen, Evan Murray, Claudia Toro, Drew R. Gentner, Cheng Huang, Shantanu Jathar, Li Li, Andrew A. May, and Allen L. Robinson
Atmos. Chem. Phys., 23, 13469–13483, https://doi.org/10.5194/acp-23-13469-2023, https://doi.org/10.5194/acp-23-13469-2023, 2023
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We update methods for calculating organic particle and vapor emissions from mobile sources in the USA. Conventionally, particulate matter (PM) and volatile organic carbon (VOC) are speciated without consideration of primary semivolatile emissions. Our methods integrate state-of-the-science speciation profiles and correct for common artifacts when sampling emissions in a laboratory. We quantify impacts of the emission updates on ambient pollution with the Community Multiscale Air Quality model.
Yanshun Li, Randall V. Martin, Chi Li, Brian L. Boys, Aaron van Donkelaar, Jun Meng, and Jeffrey R. Pierce
Atmos. Chem. Phys., 23, 12525–12543, https://doi.org/10.5194/acp-23-12525-2023, https://doi.org/10.5194/acp-23-12525-2023, 2023
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We developed and evaluated processes affecting within-day (diel) variability in PM2.5 concentrations in a chemical transport model over the contiguous US. Diel variability in PM2.5 for the contiguous US is driven by early-morning accumulation into a shallow mixed layer, decreases from mid-morning through afternoon with mixed-layer growth, increases from mid-afternoon through evening as the mixed-layer collapses, and decreases overnight as emissions decrease.
Chupeng Zhang, Shangfei Hai, Yang Gao, Yuhang Wang, Shaoqing Zhang, Lifang Sheng, Bin Zhao, Shuxiao Wang, Jingkun Jiang, Xin Huang, Xiaojing Shen, Junying Sun, Aura Lupascu, Manish Shrivastava, Jerome D. Fast, Wenxuan Cheng, Xiuwen Guo, Ming Chu, Nan Ma, Juan Hong, Qiaoqiao Wang, Xiaohong Yao, and Huiwang Gao
Atmos. Chem. Phys., 23, 10713–10730, https://doi.org/10.5194/acp-23-10713-2023, https://doi.org/10.5194/acp-23-10713-2023, 2023
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New particle formation is an important source of atmospheric particles, exerting critical influences on global climate. Numerical models are vital tools to understanding atmospheric particle evolution, which, however, suffer from large biases in simulating particle numbers. Here we improve the model chemical processes governing particle sizes and compositions. The improved model reveals substantial contributions of newly formed particles to climate through effects on cloud condensation nuclei.
Xiaodong Xie, Jianlin Hu, Momei Qin, Song Guo, Min Hu, Dongsheng Ji, Hongli Wang, Shengrong Lou, Cheng Huang, Chong Liu, Hongliang Zhang, Qi Ying, Hong Liao, and Yuanhang Zhang
Atmos. Chem. Phys., 23, 10563–10578, https://doi.org/10.5194/acp-23-10563-2023, https://doi.org/10.5194/acp-23-10563-2023, 2023
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The atmospheric age of particles reflects how long particles have been formed and suspended in the atmosphere, which is closely associated with the evolution processes of particles. An analysis of the atmospheric age of PM2.5 provides a unique perspective on the evolution processes of different PM2.5 components. The results also shed lights on how to design effective emission control actions under unfavorable meteorological conditions.
Lea Fink, Matthias Karl, Volker Matthias, Sonia Oppo, Richard Kranenburg, Jeroen Kuenen, Sara Jutterström, Jana Moldanova, Elisa Majamäki, and Jukka-Pekka Jalkanen
Atmos. Chem. Phys., 23, 10163–10189, https://doi.org/10.5194/acp-23-10163-2023, https://doi.org/10.5194/acp-23-10163-2023, 2023
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The Mediterranean Sea is a heavily trafficked shipping area, and air quality monitoring stations in numerous cities along the Mediterranean coast have detected high levels of air pollutants originating from shipping emissions. The current study investigates how existing restrictions on shipping-related emissions to the atmosphere ensure compliance with legislation. Focus was laid on fine particles and particle species, which were simulated with five different chemical transport models.
Noah A. Stanton and Neil F. Tandon
Atmos. Chem. Phys., 23, 9191–9216, https://doi.org/10.5194/acp-23-9191-2023, https://doi.org/10.5194/acp-23-9191-2023, 2023
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Chemistry in Earth’s atmosphere has a potentially strong but very uncertain impact on climate. Past attempts to fully model chemistry in Earth’s troposphere (the lowest layer of the atmosphere) typically simplified the representation of Earth’s surface, which in turn limited the ability to simulate changes in climate. The cutting-edge model that we use in this study does not require such simplification, and we use it to examine the climate effects of chemical interactions in the troposphere.
Cited articles
Alfassi, Z. B.: The chemistry of free radicals: Peroxyl radicals, 1st ed., Wiley, West Sussex, England, 546 pp., 1997.
Altieri, K., Carlton, A. G., Lim, H., Turpin, B. J., and Seitzinger, S. P.: Evidence for oligomer formation in clouds: Reaction of isoprene oxidation products, Environ. Sci. Technol., 40, 4956–4960, 2006.
Altieri, K. E., Turpin, B. J., and Seitzinger, S. P.: Oligomers, organosulfates, and nitrooxy organosulfates in rainwater identified by ultra-high resolution electrospray ionization FT-ICR mass spectrometry, Atmos. Chem. Phys., 9, 2533–2542, https://doi.org/10.5194/acp-9-2533-2009, 2009.
Arakaki, T., Anastasio, C., Kuroki, Y., Nakajima, H., Okada, K., Kotani, Y., Handa, D., Azechi, S., Kimura, T., Tsuhako, A., and Miyagi, Y.: A general scavenging rate constant for reaction of hydroxyl radical with organic carbon in atmospheric waters, Environ. Sci. Technol., 47, 8196–8203, https://doi.org/10.1021/es401927b, 2013.
Atkinson, R.: Kinetics and mechanisms of the gas-phase reactions of the hydroxyl radical with organic compounds under atmospheric conditions, Chem. Rev., 86, 1, 69–201, https://doi.org/10.1021/cr00071a004, 1986.
Baboukas, E. D., Kanakidou, M., and Mihalopoulos, N.: Carboxylic acids in gas and particulate phase above the Atlantic Ocean, J. Geophys. Res.-Atmos., 105, 14459–14471, 2000.
Battino, R., Rettich, T. R., and Tominaga, T.: The solubility of oxygen and ozone in liquids, J. Phys. Chem. Ref. Data, 12, 163–178, 1983.
Bielski, B. H. J., Cabell, D. E., Arudi, R. L., and Ross, A. B.: Reactivity of HO2/O2- radicals in aqueous solution, J. Phys. Chem. Ref. Data, 14, 1041–1100, 1985.
Blanksby, S. J. and Ellison, G. B.: Bond dissociation energies of organic molecules, Acc. Chem. Res., 36, 255–263, https://doi.org/10.1021/ar020230d, 2003.
Brégonzio-Rozier, L., Siekmann, F., Giorio, C., Pangui, E., Morales, S. B., Temime-Roussel, B., Gratien, A., Michoud, V., Ravier, S., Cazaunau, M., Tapparo, A., Monod, A., and Doussin, J.-F.: Gaseous products and secondary organic aerosol formation during long term oxidation of isoprene and methacrolein, Atmos. Chem. Phys., 15, 2953–2968, https://doi.org/10.5194/acp-15-2953-2015, 2015.
Carlton, A. G., Wiedinmyer, C., and Kroll, J. H.: A review of Secondary Organic Aerosol (SOA) formation from isoprene, Atmos. Chem. Phys., 9, 4987–5005, https://doi.org/10.5194/acp-9-4987-2009, 2009.
Carter, W. P. L., Luo, D., Malkina, I. L., and Pierce, J. A.: Environmental chamber studies of atmospheric reactivities of volatile organic compounds. Effects of varying chamber and light source, California Air Resources Board Contract A032-0692, and South Coast Air Quality Management District Coordinating Research Council, Inc., Project M-9, 1995.
Chin, M. and Wine, P. H.: A temperature-dependent competitive kinetics study of the aqueous-phase reactions of OH radicals with formate, formic acid, acetate, acetic acid and hydrated formaldehyde, in: Aquatic and Surface Photochemistry, edited by: Helz, G. R., Zepp, R. G., and Crosby, D. G., Lewis Publishers, Boca Raton, 85–96, 1994.
Christensen, H., Sehested, K., and Corfitzen, H.: Reactions of hydroxyl radicals with hydrogen peroxide at ambient and elevated temperatures, J. Phys. Chem., 86, 1588–1590, https://doi.org/10.1021/j100206a023, 1982.
Denkenberger, K. A., Moffet, R. C., Holecek, J. C., Robetier, T. P., and Prather, K. A.: Real-time, single-particle measurements of oligomers in aged ambient aerosol particles, Environ. Sci. Technol., 41, 5439–5446, 2007.
Donahue, N. M., Robinson, A. L., Stanier, C. O., and Pandis, S. N.: Coupled partitioning, dilution and chemical aging of semivolatile organics, Environ. Sci. Technol., 40, 2635–2643, 2006.
Donahue, N. M., Epstein, S. A., Pandis, S. N., and Robinson, A. L.: A two-dimensional volatility basis set: 1. organic-aerosol mixing thermodynamics, Atmos. Chem. Phys., 11, 3303–3318, https://doi.org/10.5194/acp-11-3303-2011, 2011.
Donaldson, D. J. and Valsaraj, K. T.: Adsorption and reaction of trace gas-phase organic compounds on atmospheric water film surfaces: A critical review, Environ. Sci. Technol., 44, 865–873, https://doi.org/10.1021/es902720s, 2010.
Doussin, J.-F. and Monod, A.: Structure-activity relationship for the estimation of OH-oxidation rate constants of carbonyl compounds in the aqueous phase, Atmos. Chem. Phys., 13, 11625–11641, https://doi.org/10.5194/acp-13-11625-2013, 2013.
El Haddad, I., Yao Liu, Nieto-Gligorovski, L., Michaud, V., Temime-Roussel, B., Quivet, E., Marchand, N., Sellegri, K., and Monod, A.: In-cloud processes of methacrolein under simulated conditions – Part 2: Formation of secondary organic aerosol, Atmos. Chem. Phys., 9, 5107–5117, https://doi.org/10.5194/acp-9-5107-2009, 2009.
Elliot, A. J. and Buxton, G. V.: Temperature dependence of the reactions OH + O2- and OH + HO2 in water up to 200°C, J. Chem. Soc. Faraday Trans., 88, 2465–2470, 1992.
Epstein, S. A., Tapavicza, E., Furche, F., and Nizkorodov, S. A.: Direct photolysis of carbonyl compounds dissolved in cloud and fog droplets, Atmos. Chem. Phys., 13, 9461–9477, https://doi.org/10.5194/acp-13-9461-2013, 2013.
Ervens, B.: Modeling the Processing of Aerosol and Trace Gases in Clouds and Fogs, Chemical Reviews, 115, 4157–4198, https://doi.org/10.1021/cr5005887, 2015.
Ervens, B., Gligorovski, S., and Herrmann, H.: Temperature dependent rate constants for hydroxyl radical reactions with organic compounds in aqueous solution, Phys. Chem. Chem. Phys., 5, 1811–1824, 2003.
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.
Galloway, M. M., Huisman, A. J., Yee, L. D., Chan, A. W. H., Loza, C. L., Seinfeld, J. H., and Keutsch, F. N.: Yields of oxidized volatile organic compounds during the OH radical initiated oxidation of isoprene, methyl vinyl ketone, and methacrolein under high-NOx conditions, Atmos. Chem. Phys., 11, 10779–10790, https://doi.org/10.5194/acp-11-10779-2011, 2011.
Gilbert, B. C., Holmes, R. G. G., Laue, H. A. H., and Norman, R. O. C.: Electron spin resonance studies. Part L. Reactions of alkoxyl radicals generated from alkyl hydroperoxides and titanium(III) ion in aqueous solution, J. Chem. Soc., Perk. T. 2, 1047–1052, https://doi.org/10.1039/p29760001047, 1976.
Gilbert, B. C., Smith, J. R. L., Milne, E. C., Whitwood, A. C., and Taylor, P.: Kinetic and structural EPR studies of radical polymerization. Monomer, dimer, trimer and mid-chain radicals formed via the initiation of polymerization of acrylic acid and related compounds with electrophilic radicals (●OH, SO4− ● and Cl2− ●), J. Chem. Soc., Perk. T. 2, 1759–1769, https://doi.org/10.1039/p29940001759, 1994.
Guzman, M. I., Colussi, A. J., and Hoffmann, M. R.: Photoinduced oligomerization of aqueous pyruvic acid, J. Phys. Chem. A, 110, 3619–3626, 2006.
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.
Healy, R. M., Wenger, J. C., Metzger, A., Duplissy, J., Kalberer, M., and Dommen, J.: Gas/particle partitioning of carbonyls in the photooxidation of isoprene and 1,3,5-trimethylbenzene, Atmos. Chem. Phys., 8, 3215–3230, https://doi.org/10.5194/acp-8-3215-2008, 2008.
Herckes, P., Valsaraj, K. T., and Collett Jr, J. L.: A review of observations of organic matter in fogs and clouds: Origin, processing and fate, Atmos. Res., 132–133, 434–449, https://doi.org/10.1016/j.atmosres.2013.06.005, 2013.
Herrmann, H., Hoffmann, D., Schaefer, T., Bräuer, P., and Tilgner, A.: Tropospheric Aqueous-Phase Free-Radical Chemistry: Radical Sources, Spectra, Reaction Kinetics and Prediction Tools, Chem. Phys. Chem, 11, 3796–3822, https://doi.org/10.1002/cphc.201000533, 2010.
Iraci, L. T., Baker, B. M., Tyndall, G. S., and Orlando, J. J.: Measurements of the Henry's law coefficients of 2-methyl-3-buten-2-ol, methacrolein, and methylvinyl ketone, J. Atmos. Chem., 33, 321–330, 1999.
Kalberer, M., D. Paulsen, M. Sax, M. Steinbacher, J. Dommen, A. S. H. Prevot, R. Fisseha, E. Weingartner, V. Frankevich, R. Zenobi, and Baltensperger, U.: Identification of polymers as major components of atmospheric organic aerosols, Science, 303, 1659–1662, 2004.
Kampf, C. J., Waxman, E. M., Slowik, J. G., Dommen, J., Pfaffenberger, L., Praplan, A. P., Prévôt, A. S. H., Baltensperger, U., Hoffmann, T., and Volkamer, R.: Effective Henry's Law Partitioning and the Salting Constant of Glyoxal in Aerosols Containing Sulfate, Environ. Sci. Technol., 47, 4236–4244, https://doi.org/10.1021/es400083d, 2013.
Kanakidou, M., Seinfeld, J. H., Pandis, S. N., Barnes, I., Dentener, F. J., Facchini, M. C., Van Dingenen, R., Ervens, B., Nenes, A., Nielsen, C. J., Swietlicki, E., Putaud, J. P., Balkanski, Y., Fuzzi, S., Horth, J., Moortgat, G. K., Winterhalter, R., Myhre, C. E. L., Tsigaridis, K., Vignati, E., Stephanou, E. G., and Wilson, J.: Organic aerosol and global climate modelling: a review, Atmos. Chem. Phys., 5, 1053–1123, https://doi.org/10.5194/acp-5-1053-2005, 2005.
Kawamura, K., Okuzawa, K., Aggarwal, S. G., Irie, H., Kanaya, Y., and Wang, Z.: Determination of gaseous and particulate carbonyls (glycolaldehyde, hydroxyacetone, glyoxal, methylglyoxal, nonanal and decanal) in the atmosphere at Mt. Tai, Atmos. Chem. Phys., 13, 5369–5380, https://doi.org/10.5194/acp-13-5369-2013, 2013.
Kroll, J. H., Ng, N. L., Murphy, S. M., Flagan, R. C., and Seinfeld, J. H.: Secondary organic aerosol formation from isoprene photooxidation under high NOx conditions, Geophys. Res. Lett., 32, L18808, https://doi.org/10.1029/2005GL023637, 2005.
Kroll, J. H., Ng, N. L., Murphy, S. M., Flagan, R. C., and Seinfeld, J. H.: Secondary organic aerosol formation from isoprene photooxidation, Environ. Sci. Technol., 40, 1869–1877, 2006.
Kuwata, M., Liu, Y., McKinney, K., and Martin, S. T.: Physical state and acidity of inorganic sulfate can regulate the production of secondary organic material from isoprene photooxidation products, Phys. Chem. Chem. Phys., 17, 5670–5678, https://doi.org/10.1039/c4cp04942j, 2015.
Kwon, B. G. and Kwon, J.-H.: Measurement of the hydroxyl radical formation from H2O2, NO3-, and Fe(III) using a continuous flow injection analysis, J. Ind. Eng. Chem. , 16, 193–199, https://doi.org/10.1016/j.jiec.2009.10.007, 2010.
Lang, W.: Setchenov coefficients for oxygen in aqueous solutions of various organic compounds, Fluid Phase Equilibr., 114, 123–133, https://doi.org/10.1016/0378-3812(95)02823-4, 1996.
Ligon, S. C., Husár, B., Wutzel, H., Holman, R., and Liska, R.: Strategies to Reduce Oxygen Inhibition in Photoinduced Polymerization, Chem. Rev., 114, 557–589, https://doi.org/10.1021/cr3005197, 2014.
Lim, Y. B., Tan, Y., Perri, M. J., Seitzinger, S. P., and Turpin, B. J.: Aqueous chemistry and its role in secondary organic aerosol (SOA) formation, Atmos. Chem. Phys., 10, 10521–10539, https://doi.org/10.5194/acp-10-10521-2010, 2010.
Lim, Y. B., Tan, Y., and Turpin, B. J.: Chemical insights, explicit chemistry, and yields of secondary organic aerosol from OH radical oxidation of methylglyoxal and glyoxal in the aqueous phase, Atmos. Chem. Phys., 13, 8651–8667, https://doi.org/10.5194/acp-13-8651-2013, 2013.
Lind, J. A. and Kok, G. L.: Henry's law Determinations for aqueous solutions of hydrogen peroxide, methylhydroperoxide and peroxyacetic acid, J. Geophys. Res., 91, 7889–7895, 1986.
Liu, Y., El Haddad, I., Scarfogliero, M., Nieto-Gligorovski, L., Temime-Roussel, B., Quivet, E., Marchand, N., Picquet-Varrault, B., and Monod, A.: In-cloud processes of methacrolein under simulated conditions – Part 1: Aqueous phase photooxidation, Atmos. Chem. Phys., 9, 5093–5105, https://doi.org/10.5194/acp-9-5093-2009, 2009.
Liu, Y., Monod, A., Tritscher, T., Praplan, A. P., DeCarlo, P. F., Temime-Roussel, B., Quivet, E., Marchand, N., Dommen, J., and Baltensperger, U.: Aqueous phase processing of secondary organic aerosol from isoprene photooxidation, Atmos. Chem. Phys., 12, 5879–5895, https://doi.org/10.5194/acp-12-5879-2012, 2012.
Long, T. E., McGrath, J. E., and Richard, S.: Polymers, Synthesis, pp. 751–774, in: Encyclopedia of physical science and technology, Polymers, 3rd ed., edited by: Meyers, R. A., Academic Press, New York, 15453 pp., 2001.
Mackay, D. and Shiu, W. Y.: A critical review of Henry's law constants for chemicals of environmental interest, J. Phys. Chem. Ref. Data 10, 1175–1199, 1981.
Matsunaga, S. N., Kato, S., Yoshino, A., Greenberg, J. P., Kajii, Y., and Guenther, A. B.: Gas-aerosol partitioning of semi volatile carbonyls in polluted atmosphere in Hachioji, Tokyo, Geophys. Res. Lett., 32, L11805, https://doi.org/10.1029/2004gl021893, 2005.
Mazzoleni, L. R., Ehrmann, B. M., Shen, X., Marshall, A. G., and Collett, J. L.: Water-soluble atmospheric organic matter in fog: Exact masses and chemical formula identification by ultrahigh-resolution Fourier transform ion cyclotron resonance mass Spectrometry, Environ. Sci. Technol., 44, 3690–3697, https://doi.org/10.1021/es903409k, 2010.
Mead, R. N., Mullaugh, K. M., Brooks Avery, G., Kieber, R. J., Willey, J. D., and Podgorski, D. C.: Insights into dissolved organic matter complexity in rainwater from continental and coastal storms by ultrahigh resolution Fourier transform ion cyclotron resonance mass spectrometry, Atmos. Chem. Phys., 13, 4829–4838, https://doi.org/10.5194/acp-13-4829-2013, 2013.
Mead, R. N., Felix, J. D., Avery, G. B., Kieber, R. J., Willey, J. D., and Podgorski, D. C.: Characterization of CHOS compounds in rainwater from continental and coastal storms by ultrahigh resolution mass spectrometry, Atmos. Environ., 105, 162–168, https://doi.org/10.1016/j.atmosenv.2015.01.057, 2015.
Mendez, M., Ciuraru, R., Gosselin, S., Batut, S., Visez, N., and Petitprez, D.: Reactivity of chlorine radical with submicron palmitic acid particles: kinetic measurements and product identification, Atmos. Chem. Phys., 13, 11661–11673, https://doi.org/10.5194/acp-13-11661-2013, 2013.
Michaud, V., El Haddad, I., Yao Liu, Sellegri, K., Laj, P., Villani, P., Picard, D., Marchand, N., and Monod, A.: In-cloud processes of methacrolein under simulated conditions – Part 3: Hygroscopic and volatility properties of the formed secondary organic aerosol, Atmos. Chem. Phys., 9, 5119–5130, https://doi.org/10.5194/acp-9-5119-2009, 2009.
Monod, A., Chebbi, A., Durand-Jolibois, R., and Carlier, P.: Oxidation of methanol by hydroxyl radicals in aqueous solution under simulated cloud droplet conditions, Atmos. Environ., 34, 5283–5294, 2000.
Monod, A., Poulain, L., Grubert, S., Voisin, D., and Wortham, H.: Kinetics of OH-initiated oxidation of oxygenated organic compounds in the aqueous phase: new rate constants, structure-activity relationships and atmospheric implications, Atmos. Environ., 39, 7667–7688, 2005.
Monod, A., Chevallier, E., Jolibos, R. D., Doussin, J. F., Picquet-Varrault, B., and Carlier, P.: Photooxidation of methylhydroperoxide and ethylhydroperoxide in the aqueous phase under simulated cloud droplet conditions, Atmos. Environ., 41, 2412–2426, 2007.
NDRL/NIST: Solution Kinetics Database on the Web, http://kinetics.nist.gov/solution/ (last access: 18 May 2015), 2002.
Neta, P., Huie, R. E., and Ross, A. B.: Rate constants for reactions of peroxyl radicals in fluid solutions, J. Phys. Chem. Ref. Data, 19, 413–513, 1990.
Noziere, B., Voisin, D., Longfellow, C. A., Friedli, H., Henry, B. E., and Hanson, D. R.: The uptake of methyl vinyl ketone, methacrolein, and 2-methyl-3-butene-2-ol onto sulfuric acid solutions, J. Phys. Chem. A, 110, 2387–2395, 2006.
Noziere, B., Dziedzic, P., and Cordova, A.: Inorganic ammonium salts and carbonate salts are efficient catalysts for aldol condensation in atmospheric aerosols, Phys. Chem. Chem. Phys., 12, 3864–3872, 2010.
Odian, G.: Principles of Polymerization, John Wiley & Sons Inc., Hoboken, New Jersey, 835 pp., 2004.
Odum, J. R., Hoffmann, T., Bowman, F., Collins, D., Flagan, R. C., and Seinfeld, J. H.: Gas/particle partitioning and secondary organic aerosol yields, Environ. Sci. Technol., 30, 2580–2585, 1996.
Paasivirta, J., Sinkkonen, S., Mikkelson, P., Rantio, T., and Wania, F.: Estimation of Vapor Pressures, Solubilities and Henry's Law Constants of selected persistent organic Pollutants as Functions of Temperature, Chemosphere, 39, 811–832, 1999.
Polidori, A., Turpin, B. J., Davidson, C. I., Rodenburg, L. A., and Maimone, F.: Organic PM2.5: Fractionation by polarity, FTIR Spectroscopy, and OM/OC ratio for the Pittsburgh aerosol, Aer. Sci. Tech., 42, 233–246, 2008.
Reed-Harris, A., Ervens, B., Shoemaker, R. K., Griffith, E. C., Rapf, R. J., Kroll, J., Monod, A., and Vaida, V.: Photochemical kinetics of pyruvic acid in aqueous solution, J. Phys. Chem. A, 118, 8505–8516, 2014.
Renard, P., Siekmann, F., Gandolfo, A., Socorro, J., Salque, G., Ravier, S., Quivet, E., Clément, J.-L., Traikia, M., Delort, A.-M., Voisin, D., Vuitton, V., Thissen, R., and Monod, A.: Radical mechanisms of methyl vinyl ketone oligomerization through aqueous phase OH-oxidation: on the paradoxical role of dissolved molecular oxygen, Atmos. Chem. Phys., 13, 6473–6491, https://doi.org/10.5194/acp-13-6473-2013, 2013.
Renard, P., Siekmann, F., Salque, G., Demelas, C., Coulomb, B., Vassalo, L., Ravier, S., Temime-Roussel, B., Voisin, D., and Monod, A.: Aqueous-phase oligomerization of methyl vinyl ketone through photooxidation – Part 1: Aging processes of oligomers, Atmos. Chem. Phys., 15, 21–35, https://doi.org/10.5194/acp-15-21-2015, 2015.
Sander, R.: Compilation of Henry's law constants (version 4.0) for water as solvent, Atmos. Chem. Phys., 15, 4399–4981, https://doi.org/10.5194/acp-15-4399-2015, 2015.
Schaefer, T., Schindelka, J., Hoffmann, D., and Herrmann, H.: Laboratory kinetic and mechanistic studies on the OH-initiated oxidation of acetone in aqueous solution, J. Phys. Chem. A, 116, 6317–6326, https://doi.org/10.1021/jp2120753, 2012.
Schaefer, T., van Pinxteren, D., and Herrmann, H.: Multiphase Chemistry of Glyoxal: Revised Kinetics of the Alkyl Radical Reaction with Molecular Oxygen and the Reaction of Glyoxal with OH, NO3, and SO4 – in Aqueous Solution, Environ. Sci. Technol., 49, 343–350, https://doi.org/10.1021/es505860s, 2015.
Schöne, L. and Herrmann, H.: Kinetic measurements of the reactivity of hydrogen peroxide and ozone towards small atmospherically relevant aldehydes, ketones and organic acids in aqueous solutions, Atmos. Chem. Phys., 14, 4503–4514, https://doi.org/10.5194/acp-14-4503-2014, 2014.
Schöne, L., Schindelka, J., Szeremeta, E., Schaefer, T., Hoffmann, D., Rudzinski, K. J., Szmigielski, R., and Herrmann, H.: Atmospheric aqueous phase radical chemistry of the isoprene oxidation products methacrolein, methyl vinyl ketone, methacrylic acid and acrylic acid - kinetics and product studies, Phys. Chem. Chem. Phys., 16, 6257–6272, https://doi.org/10.1039/c3cp54859g, 2014.
Schuchmann, H.-P. and von Sonntag, C.: Photolysis at 185 nm of dimethyl ether in aqueous solution: involvement of the hydroxymethyl radical, J. Photochem., 16, 289–295,https://doi.org/10.1016/0047-2670(81)80051-2, 1981.
Schuchmann, H.-P. and von Sonntag, C.: Methylperoxyl Radicals: A Study o f the y-Radiolysis of Methane in Oxygenated Aqueous Solutions, Z. Naturforschung, 39b, 217–221, 1984.
Schwartz, S.: Mass transport considerations pertinent to aqueous phase reactions of gases in liquid water clouds, in: Chemistry of Multiphase Atmospheric Systems, edited by: Jaeschke, W., NATO ASI Series, Springer, Berlin, 415–471, 1986.
Stefan, M. I. and Bolton, J. R.: Reinvestigation of the acetone degradation mechanism in dilute aqueous solution by the UV/H2O2 process, Environ. Sci. Technol., 33, 870–873, 1999.
Surratt, J. D., Murphy, S. M., Kroll, J. H., Ng, N. L., Hildebrandt, L., Sorooshian, A., Szmigielski, R., Vermeylen, R., Maenhaut, W., Claeys, M., Flagan, R. C., and Seinfeld, J. H.: Chemical composition of secondary organic aerosol formed from the photooxidation of isoprene, J. Phys. Chem. A, 110, 31, 9665–9690, https://doi.org/10.1021/jp061734m, 2006.
Tolocka, M. P., Jang, M., Ginter, J. M., Cox, F. J., Kamens, R. M., and Johnston, M. J.: Formation of oligomers in secondary organic aerosol, Environ. Sci. Technol., 38, 1428–1434, 2004.
Trump, E. R. and Donahue, N. M: Oligomer formation within secondary organic aerosols: equilibrium and dynamic considerations, Atmos. Chem. Phys., 14, 3691–3701, https://doi.org/10.5194/acp-14-3691-2014, 2014.
von Sonntag, C. and Schuchmann, H.-P.: Peroxyl radicals in aqueous solution, in: Peroxyl Radicals, edited by: Alfassi, Z. B., Wiley, Chichester, 173–234, 1997.
Wang, C., Lei, Y. D., Endo, S., and Wania, F.: Measuring and Modeling the Salting-out Effect in Ammonium Sulfate Solutions, Environ. Sci. Technol., 48, 13238–13245, https://doi.org/10.1021/es5035602, 2014.
Zhang, H. and Ying, Q.: Secondary organic aerosol formation and source apportionment in Southeast Texas, Atmos. Environ. , 45, 3217–3227, https://doi.org/10.1016/j.atmosenv.2011.03.046, 2011.
Zhang, Q., Jimenez, J. L., Canagaratna, M. R., Allan, J. D., Coe, H., Ulbrich, I., Alfarra, M. R., Takami, A., Middlebrook, A. M., Sun, Y. L., Dzepina, K., Dunlea, E., Docherty, K., DeCarlo, P. F., Salcedo, D., Onasch, T., Jayne, J. T., Miyoshi, T., Shimono, A., Hatekayama, S., Takegawa, N., Kondo, Y., Schneider, J., Drewnick, F., Borrmann, S., Weiner, S., Demerijan, K., Williams, P., Bower, K., Bahreini, R., Cottrell, L., Griffin, R. J., Rautiainen, J., Sun, J. Y., Zhang, Y. M., and Worsnop, D. R.: Ubiquity and dominance of oxygenated species in organic aerosols in anthropogenically-influenced Northern Hemisphere midlatitudes, Geophys. Res. Lett., 34, L13801, https://doi.org/10.1029/2007GL029979, 2007.
Zhang, X., Chen, Z. M., and Zhao, Y.: Laboratory simulation for the aqueous OH-oxidation of methyl vinyl ketone and methacrolein: significance to the in-cloud SOA production, Atmos. Chem. Phys., 10, 9551–9561, https://doi.org/10.5194/acp-10-9551-2010, 2010.
Short summary
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.
A detailed chemical mechanism is developed based on laboratory studies that predicts the...
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