Articles | Volume 22, issue 22
https://doi.org/10.5194/acp-22-14529-2022
© 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-22-14529-2022
© Author(s) 2022. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
16 Nov 2022
Research article |
| 16 Nov 2022
| 16 Nov 2022
Oligomer formation from the gas-phase reactions of Criegee intermediates with hydroperoxide esters: mechanism and kinetics
Long Chen
State Key Lab of Loess and Quaternary Geology (SKLLQG), Institute of Earth Environment, Chinese Academy of Sciences (CAS), Xi'an 710061, China
CAS Center for Excellence in Quaternary Science and Global Change, Xi'an 710061, China
Yu Huang
CORRESPONDING AUTHOR
State Key Lab of Loess and Quaternary Geology (SKLLQG), Institute of Earth Environment, Chinese Academy of Sciences (CAS), Xi'an 710061, China
CAS Center for Excellence in Quaternary Science and Global Change, Xi'an 710061, China
Yonggang Xue
State Key Lab of Loess and Quaternary Geology (SKLLQG), Institute of Earth Environment, Chinese Academy of Sciences (CAS), Xi'an 710061, China
CAS Center for Excellence in Quaternary Science and Global Change, Xi'an 710061, China
Zhihui Jia
School of Materials Science and Engineering, Shaanxi Normal University, Xi'an, Shaanxi 710119, China
Wenliang Wang
School of Chemistry and Chemical Engineering, Key Laboratory for Macromolecular Science of Shaanxi Province, Shaanxi Normal University, Xi'an, Shaanxi 710119, China
Related authors
Long Chen, Yu Huang, Yonggang Xue, Zhihui Jia, and Wenliang Wang
Atmos. Chem. Phys., 22, 3693–3711, https://doi.org/10.5194/acp-22-3693-2022, https://doi.org/10.5194/acp-22-3693-2022, 2022
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Quantum chemical methods are applied to gain insight into the detailed mechanisms of OH-initiated oxidation of distinct HHPs. The dominant pathway is H-abstraction from the -OOH group in the initiation reactions of the OH radical with HOCH2OOH and HOC(CH3)2OOH. H-abstraction from -CH group is competitive with that from the -OOH group in the reaction of the OH radical with HOCH(CH3)OOH. The barrier of H-abstraction from the -OOH group is slightly increased as the methyl group number increases.
Yonggang Xue, Yu Huang, Steven Sai Hang Ho, Long Chen, Liqin Wang, Shuncheng Lee, and Junji Cao
Atmos. Chem. Phys., 20, 5425–5436, https://doi.org/10.5194/acp-20-5425-2020, https://doi.org/10.5194/acp-20-5425-2020, 2020
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Particulate active metallic oxides in dust were proposed to influence the photochemical reactions of ambient volatile organic compounds (VOCs). A case study investigated the origin and transformation of VOCs during a windblown dust-to-haze pollution episode. In the dust event, a sharp decrease in VOC loading and aging of their components was observed. An increase in Ti and Fe and a fast decrease in trans-/cis-2-butene ratios demonstrated that dust can accelerate the oxidation of ambient VOCs.
Long Chen, Yu Huang, Yonggang Xue, Zhenxing Shen, Junji Cao, and Wenliang Wang
Atmos. Chem. Phys., 19, 4075–4091, https://doi.org/10.5194/acp-19-4075-2019, https://doi.org/10.5194/acp-19-4075-2019, 2019
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The present calculations show that the sequential addition of CIs to HHPs affords oligomers containing CIs as chain units. The addition of an –OOH group in HHPs to the central carbon atom of CIs is identified as the most energetically favorable channel, with a barrier height strongly dependent on both CI substituent number (one or two) and position (syn- or anti-). In particular, the introduction of a methyl group into the anti-position significantly increases the rate coefficient.
Meng Wang, Yusen Duan, Wei Xu, Qiyuan Wang, Zhuozhi Zhang, Qi Yuan, Xinwei Li, Shuwen Han, Haijie Tong, Juntao Huo, Jia Chen, Shan Gao, Zhongbiao Wu, Long Cui, Yu Huang, Guangli Xiu, Junji Cao, Qingyan Fu, and Shun-cheng Lee
Atmos. Chem. Phys., 22, 12789–12802, https://doi.org/10.5194/acp-22-12789-2022, https://doi.org/10.5194/acp-22-12789-2022, 2022
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In this study, we report the long-term measurement of organic carbon (OC) and elementary carbon (EC) in PM2.5 with hourly time resolution conducted at a regional site in Shanghai from 2016 to 2020. The results from this study provide critical information about the long-term trend of carbonaceous aerosol, in particular secondary OC, in one of the largest megacities in the world and are helpful for developing pollution control measures from a long-term planning perspective.
Long Chen, Yu Huang, Yonggang Xue, Zhihui Jia, and Wenliang Wang
Atmos. Chem. Phys., 22, 3693–3711, https://doi.org/10.5194/acp-22-3693-2022, https://doi.org/10.5194/acp-22-3693-2022, 2022
Short summary
Short summary
Quantum chemical methods are applied to gain insight into the detailed mechanisms of OH-initiated oxidation of distinct HHPs. The dominant pathway is H-abstraction from the -OOH group in the initiation reactions of the OH radical with HOCH2OOH and HOC(CH3)2OOH. H-abstraction from -CH group is competitive with that from the -OOH group in the reaction of the OH radical with HOCH(CH3)OOH. The barrier of H-abstraction from the -OOH group is slightly increased as the methyl group number increases.
Yonggang Xue, Yu Huang, Steven Sai Hang Ho, Long Chen, Liqin Wang, Shuncheng Lee, and Junji Cao
Atmos. Chem. Phys., 20, 5425–5436, https://doi.org/10.5194/acp-20-5425-2020, https://doi.org/10.5194/acp-20-5425-2020, 2020
Short summary
Short summary
Particulate active metallic oxides in dust were proposed to influence the photochemical reactions of ambient volatile organic compounds (VOCs). A case study investigated the origin and transformation of VOCs during a windblown dust-to-haze pollution episode. In the dust event, a sharp decrease in VOC loading and aging of their components was observed. An increase in Ti and Fe and a fast decrease in trans-/cis-2-butene ratios demonstrated that dust can accelerate the oxidation of ambient VOCs.
Long Chen, Yu Huang, Yonggang Xue, Zhenxing Shen, Junji Cao, and Wenliang Wang
Atmos. Chem. Phys., 19, 4075–4091, https://doi.org/10.5194/acp-19-4075-2019, https://doi.org/10.5194/acp-19-4075-2019, 2019
Short summary
Short summary
The present calculations show that the sequential addition of CIs to HHPs affords oligomers containing CIs as chain units. The addition of an –OOH group in HHPs to the central carbon atom of CIs is identified as the most energetically favorable channel, with a barrier height strongly dependent on both CI substituent number (one or two) and position (syn- or anti-). In particular, the introduction of a methyl group into the anti-position significantly increases the rate coefficient.
Jian Sun, Zhenxing Shen, Yu Huang, Junji Cao, Steven Sai Hang Ho, Xinyi Niu, Taobo Wang, Qian Zhang, Yali Lei, Hongmei Xu, and Hongxia Liu
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2018-36, https://doi.org/10.5194/acp-2018-36, 2018
Revised manuscript not accepted
Long Cui, Zhou Zhang, Yu Huang, Shun Cheng Lee, Donald Ray Blake, Kin Fai Ho, Bei Wang, Yuan Gao, Xin Ming Wang, and Peter Kwok Keung Louie
Atmos. Meas. Tech., 9, 5763–5779, https://doi.org/10.5194/amt-9-5763-2016, https://doi.org/10.5194/amt-9-5763-2016, 2016
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In this manuscript, the effect of ambient RH and T on HCHO measurements by PTR-MS was investigated, and the Poly 2-D regression was found to be a good nonlinear surface simulation of R (RH, T) for correcting measured HCHO concentration. Intercomparisons between PTR-MS and other OVOC and VOC measuring techniques were conducted through a field study in urban roadside areas of Hong Kong primarily, and good agreements were found between these different techniques.
Miriam Elser, Ru-Jin Huang, Robert Wolf, Jay G. Slowik, Qiyuan Wang, Francesco Canonaco, Guohui Li, Carlo Bozzetti, Kaspar R. Daellenbach, Yu Huang, Renjian Zhang, Zhengqiang Li, Junji Cao, Urs Baltensperger, Imad El-Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 16, 3207–3225, https://doi.org/10.5194/acp-16-3207-2016, https://doi.org/10.5194/acp-16-3207-2016, 2016
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This work represents the first online chemical characterization of the PM2.5 using a high-resolution time-of flight aerosol mass spectrometer during extreme haze events China. The application of novel source apportionment techniques allowed for an improved identification and quantification of the sources of organic aerosols. The main sources and processes driving the extreme haze events are assessed.
Related subject area
Subject: Aerosols | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Impacts of sea ice leads on sea salt aerosols and atmospheric chemistry in the Arctic
Dimethyl sulfide chemistry over the industrial era: comparison of key oxidation mechanisms and long-term observations
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
Population exposure to outdoor NO2, black carbon, and ultrafine and fine particles over Paris with multi-scale modelling down to the street scale
Predicted impacts of heterogeneous chemical pathways on particulate sulfur over Fairbanks (Alaska), the Northern Hemisphere, and the Contiguous United States
Critical load exceedances for North America and Europe using an ensemble of models and an investigation of causes of environmental impact estimate variability: an AQMEII4 study
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
Rapid oxidation of phenolic compounds by O3 and HO●: effects of the air–water interface and mineral dust in tropospheric chemical processes
Uncertainties in the effects of organic aerosol coatings on polycyclic aromatic hydrocarbon concentrations and their estimated health effects
Modeling the contribution of leads to sea spray aerosol in the high Arctic
Trends and Drivers of Soluble Iron Deposition from East Asian Dust to the Northwest Pacific: A Springtime Analysis (2001–2017)
Implications of Reduced-Complexity Aerosol Thermodynamics on Organic Aerosol Mass Concentration and Composition over North America
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
A Comprehensive Global Modelling Assessment of Nitrate Heterogeneous Formation on Desert Dust
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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
Source-resolved atmospheric metal emissions, concentrations, and deposition fluxes into the East Asian seas
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
AERO-MAP: A data compilation and modelling approach to understand spatial variability in fine and coarse mode aerosol composition
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
Spatial-temporal patterns of anthropogenic and biomass burning contributions on air pollution and mortality burden changes in India from 1995 to 2014
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
Erin J. Emme and Hannah M. Horowitz
Atmos. Chem. Phys., 25, 4531–4545, https://doi.org/10.5194/acp-25-4531-2025, https://doi.org/10.5194/acp-25-4531-2025, 2025
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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 that sea ice leads contribute to Arctic sea salt aerosols and bromine, especially in under-observed regions.
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. Winski, David G. Ferris, Karl J. Kreutz, Cameron P. Wake, and Becky Alexander
Atmos. Chem. Phys., 25, 4083–4106, https://doi.org/10.5194/acp-25-4083-2025, https://doi.org/10.5194/acp-25-4083-2025, 2025
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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 model 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.
Xiaolin Duan, Guangjie Zheng, Chuchu Chen, Qiang Zhang, and Kebin He
Atmos. Chem. Phys., 25, 3919–3928, https://doi.org/10.5194/acp-25-3919-2025, https://doi.org/10.5194/acp-25-3919-2025, 2025
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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 timescales. Its application in Changzhou, China, revealed distinct driving factors and corresponding mechanisms of aerosol acidity from annual trends to random residuals.
Wenxin Zhang, Yaman Liu, Man Yue, Xinyi Dong, Kan Huang, and Minghuai Wang
Atmos. Chem. Phys., 25, 3857–3872, https://doi.org/10.5194/acp-25-3857-2025, https://doi.org/10.5194/acp-25-3857-2025, 2025
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Understanding long-term organic aerosol (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 (SOAs) and an 8.1 % decrease in primary organic aerosols (POAs), 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.
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
Atmos. Chem. Phys., 25, 3363–3387, https://doi.org/10.5194/acp-25-3363-2025, https://doi.org/10.5194/acp-25-3363-2025, 2025
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To accurately represent the population exposure to outdoor concentrations of pollutants of interest to health (NO2, PM2.5, black carbon, and ultrafine particles), multi-scale modelling down to the street scale is set up and evaluated using measurements from field campaigns. An exposure scaling factor is defined, allowing regional-scale simulations to be corrected to evaluate population exposure. Urban heterogeneities strongly influence NO2, black carbon, and ultrafine particles but less strongly PM2.5.
Sara L. Farrell, Havala O. T. Pye, Robert Gilliam, George Pouliot, Deanna Huff, Golam Sarwar, William Vizuete, Nicole Briggs, Fengkui Duan, Tao Ma, Shuping Zhang, and Kathleen Fahey
Atmos. Chem. Phys., 25, 3287–3312, https://doi.org/10.5194/acp-25-3287-2025, https://doi.org/10.5194/acp-25-3287-2025, 2025
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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.
Paul A. Makar, Philip Cheung, Christian Hogrefe, Ayodeji Akingunola, Ummugulsum Alyuz, Jesse O. Bash, Michael D. Bell, Roberto Bellasio, Roberto Bianconi, Tim Butler, Hazel Cathcart, Olivia E. Clifton, Alma Hodzic, Ioannis Kioutsioukis, 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 W. Shephard, Ranjeet S. Sokhi, and Stefano Galmarini
Atmos. Chem. Phys., 25, 3049–3107, https://doi.org/10.5194/acp-25-3049-2025, https://doi.org/10.5194/acp-25-3049-2025, 2025
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The large range of sulfur 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 sulfur and nitrogen deposition variability. Controlling factors included the uptake of gases and aerosols by hydrometeors, aerosol inorganic chemistry, particle dry deposition, ammonia bidirectional fluxes, gas deposition via plant cuticles and soil, and land use data.
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.
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.
Sijia Lou, Manish Shrivastava, Alexandre Albinet, Sophie Tomaz, Deepchandra Srivastava, Olivier Favez, Huizhong Shen, and Aijun Ding
EGUsphere, https://doi.org/10.5194/egusphere-2024-3269, https://doi.org/10.5194/egusphere-2024-3269, 2024
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PAHs, emitted from incomplete combustion, pose serious health risks due to their carcinogenic properties. This research demonstrates that viscous organic aerosol coatings significantly hinder PAH oxidation, with spatial distributions sensitive to the degradation modelling approach. Our findings underscore the importance of accurately modelling these processes for risk assessments, highlighting the need to consider both fresh and oxidized PAHs in evaluating human exposure and health risks.
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.
Hanzheng Zhu, Yaman Liu, Man Yue, Shihui Feng, Pingqing Fu, Kan Huang, Xinyi Dong, and Minghuai Wang
EGUsphere, https://doi.org/10.5194/egusphere-2024-2293, https://doi.org/10.5194/egusphere-2024-2293, 2024
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Dust soluble iron deposition from East Asia plays an important role in the marine ecology of the Northwest Pacific. Using the developed model, our findings highlight a dual trend: a decrease in the overall deposition of soluble iron from dust, but an increase in the solubility of the iron itself due to the enhanced atmospheric processing. It underscores the critical roles of both dust emission and atmospheric processing in soluble iron deposition and marine ecology.
Camilo Serrano Damha, Kyle Gorkowski, and Andreas Zuend
EGUsphere, https://doi.org/10.5194/egusphere-2024-2712, https://doi.org/10.5194/egusphere-2024-2712, 2024
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Organic aerosol water content impacts the gas–particle partitioning of semivolatile organics. We used an aerosol thermodynamic model in the GEOS-Chem chemical transport model to efficiently account for organic aerosol water uptake and nonideal mixing. This led to a substantial enhancement in mean organic aerosol mass concentration with respect to GEOS-Chem's most advanced scheme. The water-sensitive scheme could be a valuable tool for reconciling model estimations and field measurements.
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.
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.
Ludovico Di Antonio, Matthias Beekmann, Guillaume Siour, Vincent Michoud, Christopher Cantrell, Astrid Bauville, Antonin Bergé, Mathieu Cazaunau, Servanne Chevaillier, Manuela Cirtog, Joel F. de Brito, Paola Formenti, Cecile Gaimoz, Olivier Garret, Aline Gratien, Valérie Gros, Martial Haeffelin, Lelia N. Hawkins, Simone Kotthaus, Gael Noyalet, Diana Pereira, Jean-Eudes Petit, Eva Drew Pronovost, Véronique Riffault, Chenjie Yu, Gilles Foret, Jean-François Doussin, and Claudia Di Biagio
EGUsphere, https://doi.org/10.5194/egusphere-2024-2175, https://doi.org/10.5194/egusphere-2024-2175, 2024
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Summer 2022 has been considered a proxy for future climate scenarios, given the registered hot and dry conditions. In this paper, we used the measurements from the ACROSS campaign, occurred over the Paris area in June–July 2022, in addition to observations from existing networks, to evaluate the WRF–CHIMERE model simulation over France and the Ile-de-France regions. Results over the Ile–de–France show to be satisfactory, allowing to explain the gas and aerosol variability at the ACROSS sites.
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.
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.
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.
Natalie M. Mahowald, Longlei Li, Julius Vira, Marje Prank, Douglas S. Hamilton, Hitoshi Matsui, Ron L. Miller, Louis Lu, Ezgi Akyuz, Daphne Meidan, Peter G. Hess, Heikki Lihavainen, Christine Wiedinmyer, Jenny Hand, Maria Grazia Alaimo, Célia Alves, Andres Alastuey, Paulo Artaxo, Africa Barreto, Francisco Barraza, Silvia Becagli, Giulia Calzolai, Shankararaman Chellam, Ying Chen, Patrick Chuang, David D. Cohen, Cristina Colombi, Evangelia Diapouli, Gaetano Dongarra, Konstantinos Eleftheriadis, Johann Engelbrecht, Corinne Galy-Lacaux, Cassandra Gaston, Dario Gomez, Yenny González Ramos, Roy M. Harrison, Chris Heyes, Barak Herut, Philip Hopke, Christoph Hüglin, Maria Kanakidou, Zsofia Kertesz, Zbigniew Klimont, Katriina Kyllönen, Fabrice Lambert, Xiaohong Liu, Remi Losno, Franco Lucarelli, Willy Maenhaut, Beatrice Marticorena, Randall V. Martin, Nikolaos Mihalopoulos, Yasser Morera-Gomez, Adina Paytan, Joseph Prospero, Sergio Rodríguez, Patricia Smichowski, Daniela Varrica, Brenna Walsh, Crystal Weagle, and Xi Zhao
EGUsphere, https://doi.org/10.5194/egusphere-2024-1617, https://doi.org/10.5194/egusphere-2024-1617, 2024
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Aerosol particles are an important part of the Earth system, but their concentrations are spatially and temporally heterogeneous, as well as variable in size and composition. Here we present a new compilation of PM2.5 and PM10 aerosol observations, focusing on the spatial variability across different observational stations, including composition, and demonstrate a method for comparing the datasets to model output.
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.
Bin Luo, Yuqiang Zhang, Tao Tang, Hongliang Zhang, Jianlin Hu, Jiangshan Mu, Wenxing Wang, and Likun Xue
EGUsphere, https://doi.org/10.5194/egusphere-2024-974, https://doi.org/10.5194/egusphere-2024-974, 2024
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India is facing a severe air pollution crisis that poses significant health risks, particularly from PM2.5 and O3. Our study reveals rising levels of both pollutants from 1995 to 2014, leading to increased premature mortality. While anthropogenic emissions play a significant role, biomass burning also impacts air quality, in particular seasons and regions in India. This study highlights the urgent need for localized policies to protect public health amid escalating environmental challenges.
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.
Cited articles
Alecu, I. M., Zheng, J., Zhao, Y., and Truhlar, D. G.: Computational
thermochemistry: scale factor databases and scale factors for vibrational
frequencies obtained from electronic model chemistries, J. Chem. Theory
Comput., 6, 2872–2887, https://doi.org/10.1021/ct100326h, 2010.
Anglada, J. M. and Solé, A.: Impact of the water dimer on the
atmospheric reactivity of carbonyl oxides, Phys. Chem. Chem. Phys., 18,
17698–17712, https://doi.org/10.1039/C6CP02531E, 2016.
Aplincourt, P. and Ruiz-López, M. F.: Theoretical study of formic acid
anhydride formation from carbonyl oxide in the atmosphere, J. Phys. Chem. A,
104, 380–388, https://doi.org/10.1021/jp9928208, 2000.
Atkinson, R. and Arey, J.: Atmospheric degradation of volatile organic
compounds, Chem. Rev., 103, 4605–4638, https://doi.org/10.1021/cr0206420,
2003.
Bao, J. L. and Truhlar, D. G.: Variational transition state theory:
theoretical framework and recent developments, Chem. Soc. Rev., 46,
7548–7596, https://doi.org/10.1039/c7cs00602k, 2017.
Barber, V. P., Pandit, S., Green, A. M., Trongsiriwat, N., Walsh, P. J.,
Klippenstein, S. J., and Lester, M. I.: Four-carbon Criegee intermediate
from isoprene ozonolysis: methyl vinyl ketone oxide synthesis, infrared
spectrum, and OH production, J. Am. Chem. Soc., 140, 10866–10880,
https://doi.org/10.1021/jacs.8b06010, 2018.
Boys, S. F. and Bernardi, F.: The calculation of small molecular
interactions by the differences of separate total energies. Some procedures
with reduced errors, Mol. Phys., 19, 553–566,
https://doi.org/10.1080/00268977000101561, 1970.
Cabezas, C. and Endo, Y.: The reactivity of the Criegee intermediate
CH3CHOO with water probed by FTMW spectroscopy, J. Chem. Phys., 148,
014308–014315, https://doi.org/10.1063/1.5009033, 2018.
Cabezas, C. and Endo, Y.: The Criegee intermediate-formic acid reaction
explored by rotational spectroscopy, Phys. Chem. Chem. Phys., 21,
18059–18064, https://doi.org/10.1039/c9cp03001h, 2019.
Cabezas, C. and Endo, Y.: Observation of hydroperoxyethyl formate from the
reaction between the methyl Criegee intermediate and formic acid, Phys.
Chem. Chem. Phys., 22, 446–454, https://doi.org/10.1039/C9CP05030B, 2020.
Canneaux, S., Bohr, F., and Henon, E.: KiSThelP: a program to predict
thermodynamic properties and rate constants from quantum chemistry results,
J. Comput. Chem., 35, 82–93, https://doi.org/10.1002/jcc.23470, 2013.
Caravan, R. L., Vansco, M. F., Au, K., Khan, M. A. H., Li, Y. L., Winiberg,
F. A. F., Zuraski, K., Lin, Y. H., Chao, W., Trongsiriwat, N., Walsh, P. J.,
Osborn, D. L., Percival, C. J., Lin, J. J. M., Shallcross, D. E., Sheps, L.,
Klippenstein, S. J., Taatjes, C. A., and Lester, M. I.: Direct kinetic
measurements and theoretical predictions of an isoprene-derived Criegee
intermediate, P. Natl. Acad. Sci. USA, 117, 9733–9740,
https://doi.org/10.1073/pnas.1916711117, 2020.
Chaliyakunnel, S., Millet, D. B., Wells, K. C., Cady-Pereira, K. E., and
Shephard, M. W.: A large underestimate of formic acid from tropical fires:
constraints from space-borne measurements, Environ. Sci. Technol., 50,
5631–5640, https://doi.org/10.1021/acs.est.5b06385, 2016.
Chao, W., Hsieh, J. T., Chang, C. H., and Lin, J. J. M.: Direct kinetic
measurement of the reaction of the simplest Criegee intermediate with water
vapor, Science, 347, 751–754, https://doi.org/10.1126/science.1261549, 2015.
Chen, L., Wang, W., Wang, W., Liu, Y., Liu, F., Liu, N., and Wang, B:
Water-catalyzed decomposition of the simplest Criegee intermediate
CH2OO, Theor. Chem. Acc., 135, 131–143,
https://doi.org/10.1007/s00214-016-1894-9, 2016.
Chen, L., Huang, Y., Xue, Y., Cao, J., and Wang, W.: Competition between
HO2 and H2O2 reactions with CH2OO/anti-CH3CHOO in the
oligomer formation: a theoretical perspective, J. Phys. Chem. A, 121,
6981–6991, https://doi.org/10.1021/acs.jpca.7b05951, 2017.
Chen, L., Huang, Y., Xue, Y., Cao, J., and Wang, W.: Effect of
oligomerization reactions of Criegee intermediate with organic acid/peroxy
radical on secondary organic aerosol formation from isoprene ozonolysis,
Atmos. Environ., 187, 218–229,
https://doi.org/10.1016/j.atmosenv.2018.06.001, 2018.
Chen, L., Huang, Y., Xue, Y., Shen, Z., Cao, J., and Wang, W.: Mechanistic and kinetics investigations of oligomer formation from Criegee intermediate reactions with hydroxyalkyl hydroperoxides, Atmos. Chem. Phys., 19, 4075–4091, https://doi.org/10.5194/acp-19-4075-2019, 2019.
Chhantyal-Pun, R., McGillen, M. R., Beames, J. M., Khan, M. A. H., Percival,
C. J., Shallcross, D. E., and Orr-Ewing, A. J.: Temperature Dependence of
the Rates of Reaction of Trifluoracetic Acid with Criegee Intermediates,
Angew. Chem. Int. Edit., 129, 9172–9175,
https://doi.org/10.1002/anie.201703700, 2017.
Chhantyal-Pun, R., Rotavera, B., Mcgillen, M. R., Khan, M. A. H., Eskola, A.
J., Caravan, R. L., Blacker, L., Tew, D. P., Osborn, D. L., Percival, C. J.,
Taatjes, C. A., Shallcross D. E., and Orr-Ewing, A. J.: Criegee intermediate
reactions with carboxylic acids: a potential source of secondary organic
aerosol in the atmosphere, ACS Earth Space Chem., 2, 833–842,
https://doi.org/10.1021/acsearthspacechem.8b00069, 2018.
Chung, C. A., Su, J. W., and Lee, Y. P.: Detailed mechanism and kinetics of
the reaction of Criegee intermediate CH2OO with HCOOH investigated via
infrared identification of conformers of hydroperoxymethyl formate and
formic acid anhydride, Phys. Chem. Chem. Phys., 21, 21445–21455,
https://doi.org/10.1039/c9cp04168k, 2019.
Compernolle, S., Ceulemans, K., and Müller, J.-F.: EVAPORATION: a new vapour pressure estimation methodfor organic molecules including non-additivity and intramolecular interactions, Atmos. Chem. Phys., 11, 9431–9450, https://doi.org/10.5194/acp-11-9431-2011, 2011.
Criegee, R.: Mechanism of ozonolysis, Angew. Chem. Int. Edit., 14,
745–752, https://doi.org/10.1002/anie.197507451, 1975.
Donahue, N. M., Kroll, J. H., Pandis, S. N., and Robinson, A. L.: A two-dimensional volatility basis set – Part 2: Diagnostics of organic-aerosol evolution, Atmos. Chem. Phys., 12, 615–634, https://doi.org/10.5194/acp-12-615-2012, 2012.
Drozd, G. T., Kurtén, T., Donahue, N. M., and Lester, M. I.:
Unimolecular decay of the dimethyl-substituted Criegee intermediate in
alkene ozonolysis: decay time scales and the importance of tunneling, J.
Phys. Chem. A, 121, 6036–6045, https://doi.org/10.1021/acs.jpca.7b05495,
2017.
Eckart, C.: The penetration of a potential barrier by electrons, Phys. Rev.,
35, 1303–1309, https://doi.org/10.1103/PhysRev.35.1303, 1930.
Fukui, K.: The path of chemical reactions – the IRC approach, Accounts Chem.
Res., 14, 363–368, https://doi.org/10.1021/ar00072a001, 1981.
Giorio, C., Campbell, S. J., Bruschi, M., Tampieri, F., Barbon, A.,
Toffoletti, A., Tapparo, A., Paijens, C., Wedlake, A. J., Grice, P., Howe,
D. J., and Kalbere, M.: Online quantification of Criegee intermediates of
α-pinene ozonolysis by stabilization with spin traps and
proton-transfer reaction mass spectrometry detection, J. Am. Chem. Soc.,
139, 3999–4008, https://doi.org/10.1021/jacs.6b10981, 2017.
Gong, Y. and Chen, Z.: Quantification of the role of stabilized Criegee intermediates in the formation of aerosols in limonene ozonolysis, Atmos. Chem. Phys., 21, 813–829, https://doi.org/10.5194/acp-21-813-2021, 2021.
Hammond, G. S.: A correlation of reaction rates, J. Am. Chem. Soc., 77,
334–338, https://doi.org/10.1021/ja01607a027, 1955.
Huang, H. L., Chao, W., and Lin, J. J. M.: Kinetics of a Criegee
intermediate that would survive high humidity and may oxidize atmospheric
SO2, P. Natl. Acad. Sci. USA, 112, 10857–10862, https://doi.org/10.1073/pnas.1513149112, 2015.
Humphrey, W., Dalke, A., and Schulten, K.: VMD: Visual molecular dynamics,
J. Mol. Graphics, 14, 33–38, https://doi.org/10.1016/0263-7855(96)00018-5,
1996.
Johnson, D. and Marston, G.: The gas-phase ozonolysis of unsaturated
volatile organic compounds in the troposphere, Chem. Soc. Rev., 37, 699–716,
https://doi.org/10.1039/B704260B, 2008.
Johnson, D., Lewin, A. G., and Marston, G.: The effect of
Criegee-intermediate scavengers on the OH yield from the reaction of ozone
with 2-methylbut-2-ene, J. Phys. Chem. A, 105, 2933–2935,
https://doi.org/10.1021/jp003975e, 2001.
Karton, A., Kettner, M., and Wild, D. A.: Sneaking up on the Criegee
intermediate from below: Predicted photoelectron spectrum of the
CH2OO− anion and W3-F12 electron affinity of CH2OO, Chem.
Phys. Lett., 585, 15–20, https://doi.org/10.1016/j.cplett.2013.08.075, 2013.
Khan, M. A. H., Percival, C. J., Caravan, R. L., Taatjes, C. A., and
Shallcross, D. E.: Criegee intermediates and their impacts on the
troposphere, Environ. Sci.-Proc. Imp., 20, 437–453,
https://doi.org/10.1039/C7EM00585G, 2018.
Lester, M. I. and Klippenstein, S. J.: Unimolecular decay of Criegee
intermediates to OH radical products: prompt and thermal decay processes,
Accounts Chem. Res., 51, 978–985, https://doi.org/10.1021/acs.accounts.8b00077,
2018.
Lin, J. J. M. and Chao, W.: Structure-dependent reactivity of Criegee
intermediates studied with spectroscopic methods, Chem. Soc. Rev., 46,
7483–7497, https://doi.org/10.1039/c7cs00336f, 2017.
Lin, X., Meng, Q., Feng, B., Zhai, Y., Li, Y., Yu, Y., Li, Z., Shan, X.,
Liu, F., Zhang, L., and Sheng, L.: Theoretical study on Criegee
intermediate's role in ozonolysis of acrylic acid, J. Phys. Chem. A, 123,
1929–1936, https://doi.org/10.1021/acs.jpca.8b11671, 2019.
Liu, F., Beames, J. M., Petit, A. S., McCoy, A. B., and Lester, M. I.:
Infrared-driven unimolecular reaction of CH3CHOO Criegee intermediates
to OH radical products, Science, 345, 1596–1598,
https://doi.org/10.1126/science.1257158, 2014.
Liu, L., Bei, N., Wu, J., Liu, S., Zhou, J., Li, X., Yang, Q., Feng, T., Cao, J., Tie, X., and Li, G.: Effects of stabilized Criegee intermediates (sCIs) on sulfate formation: a sensitivity analysis during summertime in Beijing–Tianjin–Hebei (BTH), China, Atmos. Chem. Phys., 19, 13341–13354, https://doi.org/10.5194/acp-19-13341-2019, 2019.
Long, B., Cheng, J. R., Tan, X. F., and Zhang, W. J.: Theoretical study on
the detailed reaction mechanisms of carbonyl oxide with formic acid, J. Mol.
Struc.-Theochem., 916, 159–167,
https://doi.org/10.1016/j.theochem.2009.09.028, 2009.
Long, B., Bao, J. L., and Truhlar, D. G.: Atmospheric chemistry of Criegee
intermediates: unimolecular reactions and reactions with water, J. Am. Chem.
Soc., 138, 14409–14422, https://doi.org/10.1021/jacs.6b08655, 2016.
Long, B., Bao, J. L., and Truhlar, D. G.: Unimolecular reaction of acetone
oxide and its reaction with water in the atmosphere, P. Natl. Acad. Sci.
USA, 115, 6135–6140, https://doi.org/10.1073/pnas.1804453115, 2018.
Lu, T. and Chen, F.: Multiwfn: A multifunctional wavefunction analyzer, J.
Comput. Chem., 33, 580–592, https://doi.org/10.1002/jcc.22885, 2012.
Mendes, J., Zhou, C. W., and Curran, H. J.: Theoretical chemical kinetic
study of the H-atom abstraction reactions from aldehydes and acids by H
atoms and OH, HO2, and CH3 radicals, J. Phys. Chem. A, 118,
12089–12104, https://doi.org/10.1021/jp5072814, 2014.
Neeb, P., Horie, O., and Moortgat, G. K.: The ethene-ozone reaction in the
gas phase, J. Phys. Chem. A, 102, 6778–6785,
https://doi.org/10.1021/jp981264z, 1998.
Novelli, A., Vereecken, L., Lelieveld, J., and Harder, H.: Direct
observation of OH formation from stabilised Criegee intermediates, Phys.
Chem. Chem. Phys., 16, 19941–19951, https://doi.org/10.1039/c4cp02719a,
2014.
Novelli, A., Hens, K., Tatum Ernest, C., Martinez, M., Nölscher, A. C., Sinha, V., Paasonen, P., Petäjä, T., Sipilä, M., Elste, T., Plass-Dülmer, C., Phillips, G. J., Kubistin, D., Williams, J., Vereecken, L., Lelieveld, J., and Harder, H.: Estimating the atmospheric concentration of Criegee intermediates and their possible interference in a FAGE-LIF instrument, Atmos. Chem. Phys., 17, 7807–7826, https://doi.org/10.5194/acp-17-7807-2017, 2017.
Osborn, D. L. and Taatjes, C. A.: The physical chemistry of Criegee
intermediates in the gas phase, Int. Rev. Phys. Chem., 34, 309–360,
https://doi.org/10.1080/0144235X.2015.1055676, 2015.
Paulot, F., Wunch, D., Crounse, J. D., Toon, G. C., Millet, D. B., DeCarlo, P. F., Vigouroux, C., Deutscher, N. M., González Abad, G., Notholt, J., Warneke, T., Hannigan, J. W., Warneke, C., de Gouw, J. A., Dunlea, E. J., De Mazière, M., Griffith, D. W. T., Bernath, P., Jimenez, J. L., and Wennberg, P. O.: Importance of secondary sources in the atmospheric budgets of formic and acetic acids, Atmos. Chem. Phys., 11, 1989–2013, https://doi.org/10.5194/acp-11-1989-2011, 2011.
Peltola, J., Seal, P., Inkilä, A., and Eskola, A.: Time-resolved,
broadband UV-absorption spectrometry measurements of Criegee intermediate
kinetics using a new photolytic precursor: unimolecular decomposition of
CH2OO and its reaction with formic acid, Phys. Chem. Chem. Phys., 22,
11797–11808, https://doi.org/10.1039/d0cp00302f, 2020.
Porterfield, J. P., Lee, K. L. K., Dell'Isola, V., Carroll, P. B., and
McCarthy, M. C.: Characterization of the simplest hydroperoxide ester,
hydroperoxymethyl formate, a precursor of atmospheric aerosols, Phys. Chem.
Chem. Phys., 21, 18065–18070, https://doi.org/10.1039/c9cp03466h, 2019.
Riva, M., Budisulistiorini, S. H., Zhang, Z., Gold, A., Thornton, J. A.,
Turpin, B. J., and Surratt, J. D.: Multiphase reactivity of gaseous
hydroperoxide oligomers produced from isoprene ozonolysis in the presence of
acidified aerosols, Atmos. Environ., 152, 314–322,
https://doi.org/10.1016/j.atmosenv.2016.12.040, 2017.
Sadezky, A., Winterhalter, R., Kanawati, B., Römpp, A., Spengler, B., Mellouki, A., Le Bras, G., Chaimbault, P., and Moortgat, G. K.: Oligomer formation during gas-phase ozonolysis of small alkenes and enol ethers: new evidence for the central role of the Criegee Intermediate as oligomer chain unit, Atmos. Chem. Phys., 8, 2667–2699, https://doi.org/10.5194/acp-8-2667-2008, 2008.
Sakamoto, Y., Inomata, S., and Hirokawa, J.: Oligomerization reaction of the
Criegee intermediate leads to secondary organic aerosol formation in
ethylene ozonolysis, J. Phys. Chem. A, 117, 12912–12921,
https://doi.org/10.1021/jp408672m, 2013.
Sakamoto, Y., Yajima, R., Inomatad, S., and Hirokawa, J.: Water vapour
effects on secondary organic aerosol formation in isoprene ozonolysis, Phys.
Chem. Chem. Phys., 19, 3165–3175, https://doi.org/10.1039/c6cp04521a, 2017.
Sipilä, M., Jokinen, T., Berndt, T., Richters, S., Makkonen, R., Donahue, N. M., Mauldin III, R. L., Kurtén, T., Paasonen, P., Sarnela, N., Ehn, M., Junninen, H., Rissanen, M. P., Thornton, J., Stratmann, F., Herrmann, H., Worsnop, D. R., Kulmala, M., Kerminen, V.-M., and Petäjä, T.: Reactivity of stabilized Criegee intermediates (sCIs) from isoprene and monoterpene ozonolysis toward SO2 and organic acids, Atmos. Chem. Phys., 14, 12143–12153, https://doi.org/10.5194/acp-14-12143-2014, 2014.
So, S., Wille, U., and Silva, G. D.: Atmospheric chemistry of enols: a
theoretical study of the vinyl alcohol + OH + O2 reaction
mechanism, Environ. Sci. Technol., 48, 6694–6701,
https://doi.org/10.1021/es500319q, 2014.
Stavrakou, T., Müller, J. F., Peeters, J., Razavi, A., Clarisse, L.,
Clerbaux, C., Coheur, P. F., Hurtmans, D., Mazière, M. D., Vigouroux,
C., Deutscher, N. M., Griffith, D. W. T., Jones, N., and Paton-Walsh, C.:
Satellite evidence for a large source of formic acid from boreal and
tropical forests, Nat. Geosci., 5, 26–30, https://doi.org/10.1038/ngeo1354,
2012.
Taatjes, C. A.: Criegee intermediates: what direct production and detection
can teach us about reactions of carbonyl oxides, Annu. Rev. Phys. Chem., 68,
183–207, https://doi.org/10.1146/annurev-physchem-052516-050739, 2017.
Taatjes, C. A., Welz, O., Eskola, A. J., Savee, J. D., Scheer, A. M.,
Shallcross, D. E., Rotavera, B., Lee, E. P. F., Dyke, J. M., Mok, D. K. W.,
Osborn, D. L., and Percival, C. J.: Direct measurements of
conformer-dependent reactivity of the Criegee intermediate CH3CHOO,
Science, 340, 177–180, https://doi.org/10.1126/science.1234689, 2013.
Taatjes, C. A., Khan, M. A. H., Eskola, A. J., Percival, C. J., Osborn, D.
L., Wallington, T. J., and Shallcross, D. E.: Reaction of perfluorooctanoic
acid with Criegee intermediates and implications for the atmospheric fate of
perfluorocarboxylic acids, Environ. Sci. Technol., 53, 1245–1251,
https://doi.org/10.1021/acs.est.8b05073, 2019.
Tobias, H. J. and Ziemann, P. J.: Kinetics of the gas-phase reactions of
alcohols, aldehydes, carboxylic acids, and water with the C13 stabilized
Criegee intermediate formed from ozonolysis of 1-tetradecene, J. Phys. Chem.
A, 105, 6129–6135, https://doi.org/10.1021/jp004631r, 2001.
Truhlar, D. G., Hase, W. L., and Hynes, J. T.: Current status of
transition-state theory, J. Phys. Chem., 87, 2664–2682,
https://doi.org/10.1021/jp953748q, 1996.
Vansco, M. F., Zuraski, K., Winiberg, F. A. F., Au, K., Trongsiriwat, N.,
Walsh, P. J., Osborn, D. L., Percival, C. J., Klippenstein, S. J., Taatjes,
C. A., Lester, M. I., and Caravan, R. L.: Functionalized hydroperoxide
formation from the reaction of methacrolein-oxide, an isoprene-derived
Criegee intermediate, with formic acid: experiment and theory, Molecules,
26, 3058–3072, https://doi.org/10.3390/molecules26103058, 2021.
Vereecken, L.: The reaction of Criegee intermediates with acids and enols,
Phys. Chem. Chem. Phys., 19, 28630–28640,
https://doi.org/10.1039/c7cp05132h, 2017.
Vereecken, L., Harder, H., and Novelli, A.: The reaction of Criegee
intermediates with NO, RO2, and SO2, and their fate in the
atmosphere, Phys. Chem. Chem. Phys., 14, 14682–14695,
https://doi.org/10.1039/c2cp42300f, 2012.
Wang, S., Newland, M. J., Deng, W., Rickard, A. R., Hamilton, J. F.,
Muñoz, A., Ródenas, M., Vázquez, M. M., Wang, L., and Wang, X.:
Aromatic photo-oxidation, a new source of atmospheric acidity, Environ. Sci.
Technol., 54, 7798–7806, https://doi.org/10.1021/acs.est.0c00526, 2020.
Welz, O., Savee, J. D., Osborn, D. L., Vasu, S. S., Percival, C. J.,
Shallcross, D. E., and Taatjes, C. A.: Direct kinetic measurements of
Criegee intermediate (CH2OO) formed by reaction of CH2I with
O2, Science, 335, 204–207, https://doi.org/10.1126/science.1213229,
2012.
Welz, O., Eskola, A. J., Sheps, L., Rotavera, B., Savee, J. D., Scheer, A.
M., Osborn, D. L., Lowe, D., Booth, A. M., Xiao, P., Khan, M. A. H.,
Percival, C. J., Shallcross, D. E., and Taatjes, C. A.: Rate coefficients of
C(1) and C(2) Criegee intermediate reactions with formic and acetic Acid
near the collision limit: direct kinetics measurements and atmospheric
implications, Angew. Chem. Int. Edit., 53, 4547–4550,
https://doi.org/10.1002/anie.201400964, 2014.
Yin, C. and Takahashi, K.: How does substitution affect the unimolecular
reaction rates of Criegee intermediates? Phys. Chem. Chem. Phys., 19,
12075–12084, https://doi.org/10.1039/c7cp01091e, 2017.
Yu, S.: Role of organic acids (formic, acetic, pyruvic and oxalic) in the
formation of cloud condensation nuclei (CCN): a review, Atmos. Res., 53,
185–217, https://doi.org/10.1016/S0169-8095(00)00037-5, 2000.
Zhang, P., Wang, W., Zhang, T., Chen, L., Du, Y., Li, C., and Lv, J.:
Theoretical study on the mechanism and kinetics for the self-reaction of
C2H5O2 radicals, J. Phys. Chem. A, 116, 4610–4620,
https://doi.org/10.1021/jp301308u, 2012.
Zhao, R., Kenseth, C. M., Huang, Y., Dalleska, N. F., Kuang, X. M., Chen,
J., Paulson, S. E., and Seinfeld, J. H.: Rapid aqueous-phase hydrolysis of
ester hydroperoxides arising from Criegee intermediates and organic acids,
J. Phys. Chem. A, 122, 5190–5201, https://doi.org/10.1021/acs.jpca.8b02195,
2018.
Zhao, Y. and Truhlar, D. G.: The M06 suite of density functionals for main
group thermochemistry, thermochemical kinetics, noncovalent interactions,
excited states, and transition elements: two new functionals and systematic
testing of four M06-class functionals and 12 other functionals, Theor. Chem.
Acc., 120, 215–241, https://doi.org/10.1007/s00214-007-0310-x, 2008.
Zhao, Y., Wingen, L. M., Perraud, V., Greaves, J., and Finlayson-Pitts, B.
J.: Role of the reaction of stabilized Criegee intermediates with peroxy
radicals in particle formation and growth in air, Phys. Chem. Chem. Phys.,
17, 12500–12514, https://doi.org/10.1039/c5cp01171j, 2015.
Zheng, J., Bao, L. J., Meana-Paneda, R., Zhang, S., Lynch, B. J., Corchado, J. C., Chuang, Y. Y., Fast, P. L., Hu, W. P., Liu, Y. P., Lynch, G. C., Nguyen, K. A., Jackels, C. F., Fernandez-Ramos, A., Ellingson, B. A., Melissas, V. S., Villa, J., Rossi, I., Coitino, L., Pu, J., Albu, T. V., Steckler, R., Garrett, B. C., Issacson, A. D., and Truhlar, D. G.: Polyrate, version 2017-C, University of Minnesota, Minneapolis, MN, https://comp.chem.umn.edu/polyrate/ (last access: 9 November 2022), 2018.
Zhou, S., Joudan, S., Forbes, M. W., Zhou, Z., and Abbatt, J. P. D.:
Reaction of condensed-phase Criegee intermediates with carboxylic acids and
perfluoroalkyl carboxylic acids, Environ. Sci. Tech. Let., 6, 243–250,
https://doi.org/10.1021/acs.estlett.9b00165, 2019.
Short summary
Quantum chemical methods are applied to gain insight into the oligomerization reaction mechanisms and kinetics of distinct stabilized Criegee intermediate (SCI) reactions with hydroperoxide esters, where calculations show that SCI addition reactions with hydroperoxide esters proceed through the successive insertion of SCIs to form oligomers that involve SCIs as the repeating unit. The saturated vapor pressure of the formed oligomers decreases monotonically with the increasing number of SCIs.
Quantum chemical methods are applied to gain insight into the oligomerization reaction...
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