Articles | Volume 20, issue 9
https://doi.org/10.5194/acp-20-5679-2020
© Author(s) 2020. 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-20-5679-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
13 May 2020
Research article |
| 13 May 2020
Thermodynamic properties of isoprene- and monoterpene-derived organosulfates estimated with COSMOtherm
Nano and Molecular Systems Research Unit, University of Oulu, P.O. Box 3000, 90014 Oulu, Finland
Jonas Elm
Department of Chemistry and iClimate, Aarhus University, Langelandsgade 140, 8000 Aarhus C, Denmark
Jussi Malila
Nano and Molecular Systems Research Unit, University of Oulu, P.O. Box 3000, 90014 Oulu, Finland
Silvia M. Calderón
Nano and Molecular Systems Research Unit, University of Oulu, P.O. Box 3000, 90014 Oulu, Finland
Nano and Molecular Systems Research Unit, University of Oulu, P.O. Box 3000, 90014 Oulu, Finland
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mostly below 0.1mm.
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Related subject area
Subject: Aerosols | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Physics (physical properties and processes)
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Particle size of atmospheric aerosol is important for estimating its climate and health effects, but simulating atmospheric aerosol size is computationally demanding. This study derives a simple parameterization of the size of organic and secondary inorganic ambient aerosol that can be applied to atmospheric models. Applying this parameterization allows a better representation of the global spatial pattern of aerosol size, as verified by ground and airborne measurements.
Mengjiao Jiang, Yaoting Li, Weiji Hu, Yinshan Yang, Guy Brasseur, and Xi Zhao
Atmos. Chem. Phys., 23, 4545–4557, https://doi.org/10.5194/acp-23-4545-2023, https://doi.org/10.5194/acp-23-4545-2023, 2023
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Relatively clean background aerosol over the Tibetan Plateau makes the study of aerosol–cloud–precipitation interactions distinctive. A convection on 24 July 2014 in Naqu was selected using the Weather Research Forecasting (WRF) model, including the Thompson aerosol-aware microphysical scheme. Our study uses a compromise approach to the limited observations. We show that the transformation of cloud water to graupel and the development of convective clouds are favored in a polluted situation.
Pantelis Kiriakidis, Antonis Gkikas, Georgios Papangelis, Theodoros Christoudias, Jonilda Kushta, Emmanouil Proestakis, Anna Kampouri, Eleni Marinou, Eleni Drakaki, Angela Benedetti, Michael Rennie, Christian Retscher, Anne Grete Straume, Alexandru Dandocsi, Jean Sciare, and Vasilis Amiridis
Atmos. Chem. Phys., 23, 4391–4417, https://doi.org/10.5194/acp-23-4391-2023, https://doi.org/10.5194/acp-23-4391-2023, 2023
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With the launch of the Aeolus satellite, higher-accuracy wind products became available. This research was carried out to validate the assimilated wind products by testing their effect on the WRF-Chem model predictive ability of dust processes. This was carried out for the eastern Mediterranean and Middle East region for two 2-month periods in autumn and spring 2020. The use of the assimilated products improved the dust forecasts of the autumn season (both quantitatively and qualitatively).
Ian Chang, Lan Gao, Connor J. Flynn, Yohei Shinozuka, Sarah J. Doherty, Michael S. Diamond, Karla M. Longo, Gonzalo A. Ferrada, Gregory R. Carmichael, Patricia Castellanos, Arlindo M. da Silva, Pablo E. Saide, Calvin Howes, Zhixin Xue, Marc Mallet, Ravi Govindaraju, Qiaoqiao Wang, Yafang Cheng, Yan Feng, Sharon P. Burton, Richard A. Ferrare, Samuel E. LeBlanc, Meloë S. Kacenelenbogen, Kristina Pistone, Michal Segal-Rozenhaimer, Kerry G. Meyer, Ju-Mee Ryoo, Leonhard Pfister, Adeyemi A. Adebiyi, Robert Wood, Paquita Zuidema, Sundar A. Christopher, and Jens Redemann
Atmos. Chem. Phys., 23, 4283–4309, https://doi.org/10.5194/acp-23-4283-2023, https://doi.org/10.5194/acp-23-4283-2023, 2023
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Abundant aerosols are present above low-level liquid clouds over the southeastern Atlantic during late austral spring. The model simulation differences in the proportion of aerosol residing in the planetary boundary layer and in the free troposphere can greatly affect the regional aerosol radiative effects. This study examines the aerosol loading and fractional aerosol loading in the free troposphere among various models and evaluates them against measurements from the NASA ORACLES campaign.
Juli I. Rubin, Jeffrey S. Reid, Peng Xian, Christopher M. Selman, and Thomas F. Eck
Atmos. Chem. Phys., 23, 4059–4090, https://doi.org/10.5194/acp-23-4059-2023, https://doi.org/10.5194/acp-23-4059-2023, 2023
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This work aims to quantify the covariability between aerosol optical depth/extinction with water vapor (PW) globally, using NASA AERONET observations and NAAPS model data. Findings are important for data assimilation and radiative transfer. The study shows statistically significant and positive AOD–PW relationships are found across the globe, varying in strength with location and season and tied to large-scale aerosol events. Hygroscopic growth was also found to be an important factor.
Christopher D. Wells, Matthew Kasoar, Nicolas Bellouin, and Apostolos Voulgarakis
Atmos. Chem. Phys., 23, 3575–3593, https://doi.org/10.5194/acp-23-3575-2023, https://doi.org/10.5194/acp-23-3575-2023, 2023
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The climate is altered by greenhouse gases and air pollutant particles, and such emissions are likely to change drastically in the future over Africa. Air pollutants do not travel far, so their climate effect depends on where they are emitted. This study uses a climate model to find the climate impacts of future African pollutant emissions being either high or low. The particles absorb and scatter sunlight, causing the ground nearby to be cooler, but elsewhere the increased heat causes warming.
Geeta G. Persad
Atmos. Chem. Phys., 23, 3435–3452, https://doi.org/10.5194/acp-23-3435-2023, https://doi.org/10.5194/acp-23-3435-2023, 2023
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Human-induced aerosol pollution has major impacts on both local and global precipitation. This study demonstrates using a global climate model that both the strength and localization of aerosols' precipitation impacts are highly dependent on which region the aerosols are emitted from. The findings highlight that the geographic distribution of human-induced aerosol emissions must be accounted for when quantifying their influence on global precipitation.
Tuuli Miinalainen, Harri Kokkola, Antti Lipponen, Antti-Pekka Hyvärinen, Vijay Kumar Soni, Kari E. J. Lehtinen, and Thomas Kühn
Atmos. Chem. Phys., 23, 3471–3491, https://doi.org/10.5194/acp-23-3471-2023, https://doi.org/10.5194/acp-23-3471-2023, 2023
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We simulated the effects of aerosol emission mitigation on both global and regional radiative forcing and city-level air quality with a global-scale climate model. We used a machine learning downscaling approach to bias-correct the PM2.5 values obtained from the global model for the Indian megacity New Delhi. Our results indicate that aerosol mitigation could result in both improved air quality and less radiative heating for India.
Peng Wang, Ruhan Zhang, Shida Sun, Meng Gao, Bo Zheng, Dan Zhang, Yanli Zhang, Gregory R. Carmichael, and Hongliang Zhang
Atmos. Chem. Phys., 23, 2983–2996, https://doi.org/10.5194/acp-23-2983-2023, https://doi.org/10.5194/acp-23-2983-2023, 2023
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In China, the number of vehicles has jumped significantly in the last decade. This caused severe traffic congestion and aggravated air pollution. In this study, we developed a new temporal allocation approach to quantify the impacts of traffic congestion. We found that traffic congestion worsens air quality and the health burden across China, especially in the urban clusters. More effective and comprehensive vehicle emission control policies should be implemented to improve air quality in China.
Ruth Price, Andrea Baccarini, Julia Schmale, Paul Zieger, Ian M. Brooks, Paul Field, and Ken S. Carslaw
Atmos. Chem. Phys., 23, 2927–2961, https://doi.org/10.5194/acp-23-2927-2023, https://doi.org/10.5194/acp-23-2927-2023, 2023
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Arctic clouds can control how much energy is absorbed by the surface or reflected back to space. Using a computer model of the atmosphere we investigated the formation of atmospheric particles that allow cloud droplets to form. We found that particles formed aloft are transported to the lowest part of the Arctic atmosphere and that this is a key source of particles. Our results have implications for the way Arctic clouds will behave in the future as climate change continues to impact the region.
Kevin Ohneiser, Albert Ansmann, Jonas Witthuhn, Hartwig Deneke, Alexandra Chudnovsky, Gregor Walter, and Fabian Senf
Atmos. Chem. Phys., 23, 2901–2925, https://doi.org/10.5194/acp-23-2901-2023, https://doi.org/10.5194/acp-23-2901-2023, 2023
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This study shows that smoke layers can reach the tropopause via the self-lofting effect within 3–7 d in the absence of pyrocumulonimbus convection if the
aerosol optical thickness is larger than approximately 2 for a longer time period. When reaching the stratosphere, wildfire smoke can sensitively influence the stratospheric composition on a hemispheric scale and thus can affect the Earth’s climate and the ozone layer.
Neeldip Barman and Sharad Gokhale
EGUsphere, https://doi.org/10.5194/egusphere-2023-88, https://doi.org/10.5194/egusphere-2023-88, 2023
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The study shows that during the pre-monsoon season transported aerosols, especially from Indo-Gangetic Plains (IGP) has a greater impact w.r.t air pollution, radiative forcing and rainfall over North-East (NE) India than emissions from within NE India itself. Hence, controlling emissions in the IGP will be significantly more fruitful in reducing pollution as well as climatic impacts over this region.
Marios Chatziparaschos, Nikos Daskalakis, Stelios Myriokefalitakis, Nikos Kalivitis, Athanasios Nenes, María Gonçalves Ageitos, Montserrat Costa-Surós, Carlos Pérez García-Pando, Medea Zanoli, Mihalis Vrekoussis, and Maria Kanakidou
Atmos. Chem. Phys., 23, 1785–1801, https://doi.org/10.5194/acp-23-1785-2023, https://doi.org/10.5194/acp-23-1785-2023, 2023
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Ice formation is enabled by ice-nucleating particles (INP) at higher temperatures than homogeneous formation and can profoundly affect the properties of clouds. Our global model results show that K-feldspar is the most important contributor to INP concentrations globally, affecting mid-level mixed-phase clouds. However, quartz can significantly contribute and dominates the lowest and the highest altitudes of dust-derived INP, affecting mainly low-level and high-level mixed-phase clouds.
Chandan Sarangi, Yun Qian, L. Ruby Leung, Yang Zhang, Yufei Zou, and Yuhang Wang
Atmos. Chem. Phys., 23, 1769–1783, https://doi.org/10.5194/acp-23-1769-2023, https://doi.org/10.5194/acp-23-1769-2023, 2023
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We show that for air quality, the densely populated eastern US may see even larger impacts of wildfires due to long-distance smoke transport and associated positive climatic impacts, partially compensating the improvements from regulations on anthropogenic emissions. This study highlights the tension between natural and anthropogenic contributions and the non-local nature of air pollution that complicate regulatory strategies for improving future regional air quality for human health.
Rémy Lapere, Nicolás Huneeus, Sylvain Mailler, Laurent Menut, and Florian Couvidat
Atmos. Chem. Phys., 23, 1749–1768, https://doi.org/10.5194/acp-23-1749-2023, https://doi.org/10.5194/acp-23-1749-2023, 2023
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Glaciers in the Andes of central Chile are shrinking rapidly in response to global warming. This melting is accelerated by the deposition of opaque particles onto snow and ice. In this work, model simulations quantify typical deposition rates of soot on glaciers in summer and winter months and show that the contribution of emissions from Santiago is not as high as anticipated. Additionally, the combination of regional- and local-scale meteorology explains the seasonality in deposition.
Ju Liang and Jim Haywood
Atmos. Chem. Phys., 23, 1687–1703, https://doi.org/10.5194/acp-23-1687-2023, https://doi.org/10.5194/acp-23-1687-2023, 2023
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The recent record-breaking flood events in China during the summer of 2021 highlight the importance of mitigating the risks from future changes in high-impact weather systems under global warming. Based on a state-of-the-art Earth system model, we demonstrate a pilot study on the responses of atmospheric rivers and extreme precipitation over East Asia to anthropogenically induced climate warming and an unconventional mitigation strategy – stratospheric aerosol injection.
Azad Madhu, Myoseon Jang, and David Deacon
Atmos. Chem. Phys., 23, 1661–1675, https://doi.org/10.5194/acp-23-1661-2023, https://doi.org/10.5194/acp-23-1661-2023, 2023
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SOA formation is simulated using the UNIPAR model for series of linear alkanes. The inclusion of autoxidation reactions within the explicit gas mechanisms of C9–C12 was found to significantly improve predictions. Available product distributions were extrapolated with an incremental volatility coefficient (IVC) to predict SOA formation of alkanes without explicit mechanisms. These product distributions were used to simulate SOA formation from C13 and C15 and had good agreement with chamber data.
Jianbing Jin, Bas Henzing, and Arjo Segers
Atmos. Chem. Phys., 23, 1641–1660, https://doi.org/10.5194/acp-23-1641-2023, https://doi.org/10.5194/acp-23-1641-2023, 2023
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Aerosol models and satellite retrieval algorithms rely on different aerosol size assumptions. In practice, differences between simulations and observations do not always reflect the difference in aerosol amount. To avoid inconsistencies, we designed a hybrid assimilation approach. Different from a standard aerosol optical depth (AOD) assimilation that directly assimilates AODs, the hybrid one estimates aerosol size parameters by assimilating Ängström observations before assimilating the AODs.
Je-Yun Chun, Robert Wood, Peter Blossey, and Sarah J. Doherty
Atmos. Chem. Phys., 23, 1345–1368, https://doi.org/10.5194/acp-23-1345-2023, https://doi.org/10.5194/acp-23-1345-2023, 2023
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We investigate the impact of injected aerosol on subtropical low marine clouds under a variety of meteorological conditions using high-resolution model simulations. This study illustrates processes perturbed by aerosol injections and their impact on cloud properties (e.g., cloud number concentration, thickness, and cover). We show that those responses are highly sensitive to background meteorological conditions, such as precipitation, and background cloud properties.
Huan Yang, Ivo Neefjes, Valtteri Tikkanen, Jakub Kubečka, Theo Kurtén, Hanna Vehkamäki, and Bernhard Reischl
EGUsphere, https://doi.org/10.5194/egusphere-2022-1449, https://doi.org/10.5194/egusphere-2022-1449, 2023
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We present a new analytical model for collision rates between molecules and clusters of arbitrary sizes, that accounts for long-range interactions. The model is verified against atomistic simulations of typical acid-base clusters participating in atmospheric new particle formation. Results show that accounting for long-range interactions leads to 2–3 times higher collision rates for small clusters, indicating the necessity of including such forces in atmospheric new particle formation modelling.
Nora L. S. Fahrenbach and Massimo A. Bollasina
Atmos. Chem. Phys., 23, 877–894, https://doi.org/10.5194/acp-23-877-2023, https://doi.org/10.5194/acp-23-877-2023, 2023
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We studied the monthly-scale climate response to COVID-19 aerosol emission reductions during January–May 2020 using climate models. Our results show global temperature and rainfall anomalies driven by circulation changes. The climate patterns reverse polarity from JF to MAM due to a shift in the main SO2 reduction region from China to India. This real-life example of rapid climate adjustments to abrupt, regional aerosol emission reduction has large implications for future climate projections.
Seoung Soo Lee, Junshik Um, Won Jun Choi, Kyung-Ja Ha, Chang Hoon Jung, Jianping Guo, and Youtong Zheng
Atmos. Chem. Phys., 23, 273–286, https://doi.org/10.5194/acp-23-273-2023, https://doi.org/10.5194/acp-23-273-2023, 2023
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This paper elaborates on process-level mechanisms regarding how the interception of radiation by aerosols interacts with the surface heat fluxes and atmospheric instability in warm cumulus clouds. This paper elucidates how these mechanisms vary with the location or altitude of an aerosol layer. This elucidation indicates that the location of aerosol layers should be taken into account for parameterizations of aerosol–cloud interactions.
Meredith Schervish and Manabu Shiraiwa
Atmos. Chem. Phys., 23, 221–233, https://doi.org/10.5194/acp-23-221-2023, https://doi.org/10.5194/acp-23-221-2023, 2023
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Secondary organic aerosols (SOAs) can exhibit complex non-ideal behavior and adopt an amorphous semisolid state. We simulate condensation of semi-volatile compounds into a phase-separated particle to investigate the effect of non-ideality and particle phase state on the equilibration timescale of SOA partitioning. Our results provide useful insights into the interpretation of experimental observations and the description and treatment of SOA in aerosol models.
Christof G. Beer, Johannes Hendricks, and Mattia Righi
Atmos. Chem. Phys., 22, 15887–15907, https://doi.org/10.5194/acp-22-15887-2022, https://doi.org/10.5194/acp-22-15887-2022, 2022
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Ice-nucleating particles (INPs) have important influences on cirrus clouds and the climate system; however, their global atmospheric distribution in the cirrus regime is still very uncertain. We present a global climatology of INPs under cirrus conditions derived from model simulations, considering the mineral dust, soot, crystalline ammonium sulfate, and glassy organics INP types. The comparison of respective INP concentrations indicates the large importance of ammonium sulfate particles.
Mykhailo Savenets, Larysa Pysarenko, Svitlana Krakovska, Alexander Mahura, and Tuukka Petäjä
Atmos. Chem. Phys., 22, 15777–15791, https://doi.org/10.5194/acp-22-15777-2022, https://doi.org/10.5194/acp-22-15777-2022, 2022
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The paper explores the spatio-temporal variability of black carbon during a wildfire in August 2010, with a focus on Ukraine. As a research tool, the seamless Enviro-HIRLAM modelling system is used for investigating the atmospheric transport of aerosol particles emitted by wildfires from remote and local sources. The results of this study improve our understanding of the physical and chemical processes and the interactions of aerosols in the atmosphere.
Huilin Huang, Yun Qian, Ye Liu, Cenlin He, Jianyu Zheng, Zhibo Zhang, and Antonis Gkikas
Atmos. Chem. Phys., 22, 15469–15488, https://doi.org/10.5194/acp-22-15469-2022, https://doi.org/10.5194/acp-22-15469-2022, 2022
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Using a clustering method developed in the field of artificial neural networks, we identify four typical dust transport patterns across the Sierra Nevada, associated with the mesoscale and regional-scale wind circulations. Our results highlight the connection between dust transport and dominant weather patterns, which can be used to understand dust transport in a changing climate.
Anbao Zhu, Haiming Xu, Jiechun Deng, Jing Ma, and Shaofeng Hua
Atmos. Chem. Phys., 22, 15425–15447, https://doi.org/10.5194/acp-22-15425-2022, https://doi.org/10.5194/acp-22-15425-2022, 2022
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This study demonstrates the instant and delayed effects of biomass burning (BB) aerosols on precipitation over the Indochina Peninsula (ICP). The convection suppression due to the BB aerosol-induced stabilized atmosphere dominates over the favorable water-vapor condition induced by large-scale circulation responses, leading to an overall reduced precipitation in March, while the delayed effect promotes precipitation from early April to mid April due to the anomalous atmospheric circulations.
Wenjie Zhang, Hong Wang, Xiaoye Zhang, Liping Huang, Yue Peng, Zhaodong Liu, Xiao Zhang, and Huizheng Che
Atmos. Chem. Phys., 22, 15207–15221, https://doi.org/10.5194/acp-22-15207-2022, https://doi.org/10.5194/acp-22-15207-2022, 2022
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Aerosol–cloud interaction (ACI) is first implemented in the atmospheric chemistry system GRAPES_Meso5.1/CUACE. ACI can improve the simulated cloud, temperature, and precipitation under haze pollution conditions in Jing-Jin-Ji in China. This paper demonstrates the critical role of ACI in current numerical weather prediction over the severely polluted region.
Santeri Tuovinen, Runlong Cai, Veli-Matti Kerminen, Jingkun Jiang, Chao Yan, Markku Kulmala, and Jenni Kontkanen
Atmos. Chem. Phys., 22, 15071–15091, https://doi.org/10.5194/acp-22-15071-2022, https://doi.org/10.5194/acp-22-15071-2022, 2022
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We compare observed survival probabilities of atmospheric particles from Beijing, China, with survival probabilities based on analytical formulae and model simulations. We find observed survival probabilities under polluted conditions at smaller sizes to be higher, while at larger sizes they are lower than or similar to theoretical survival probabilities. Uncertainties in condensation sink and growth rate are unlikely to explain higher-than-predicted survival probabilities at smaller sizes.
Stephanie Woodward, Alistair A. Sellar, Yongming Tang, Marc Stringer, Andrew Yool, Eddy Robertson, and Andy Wiltshire
Atmos. Chem. Phys., 22, 14503–14528, https://doi.org/10.5194/acp-22-14503-2022, https://doi.org/10.5194/acp-22-14503-2022, 2022
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We describe the dust scheme in the UKESM1 Earth system model and show generally good agreement with observations. Comparing with the closely related HadGEM3-GC3.1 model, we show that dust differences are not only due to inter-model differences but also to the dust size distribution. Under climate change, HadGEM3-GC3.1 dust hardly changes, but UKESM1 dust decreases because that model includes the vegetation response which, in our models, has a bigger impact on dust than climate change itself.
Yang Yang, Liangying Zeng, Hailong Wang, Pinya Wang, and Hong Liao
Atmos. Chem. Phys., 22, 14489–14502, https://doi.org/10.5194/acp-22-14489-2022, https://doi.org/10.5194/acp-22-14489-2022, 2022
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Using an aerosol–climate model, dust pollution in China affected by different spatial and temporal types of El Niño are examined. Both eastern and central Pacific El Niño and short-duration El Niño increase winter dust concentrations over northern China, while long-duration El Niño decreases concentrations. Only long-duration El Niño events can significantly affect dust over China in the following spring. This study has profound implications for air pollution control and dust storm prediction.
Danny M. Leung, Jasper F. Kok, Longlei Li, Gregory S. Okin, Catherine Prigent, Martina Klose, Carlos Pérez Garcia-Pando, Laurent Menut, Natalie M. Mahowald, David M. Lawrence, and Marcelo Chamecki
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-719, https://doi.org/10.5194/acp-2022-719, 2022
Revised manuscript accepted for ACP
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Desert dust modeling is important for understanding climate change, as dust regulates the atmosphere's greenhouse effect and radiation. This study formulates and proposes a more physical and realistic desert dust emission scheme for global and regional climate models. By considering more aeolian processes in our emission scheme, our simulations match better against dust observations than existing schemes. We believe this work is vital in improving dust representation in climate models.
Robin Stevens, Andrei Ryjkov, Mahtab Majdzadeh, and Ashu Dastoor
Atmos. Chem. Phys., 22, 13527–13549, https://doi.org/10.5194/acp-22-13527-2022, https://doi.org/10.5194/acp-22-13527-2022, 2022
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Absorbing particles like black carbon can be coated with other matter. How much radiation these particles absorb depends on the coating thickness. The removal of these particles by clouds and rain depends on the coating composition. These effects are important for both climate and air quality. We implement a more detailed representation of these particles in an air quality model which accounts for both coating thickness and composition. We find a significant effect on particle concentrations.
Fan Wang, Gregory R. Carmichael, Jing Wang, Bin Chen, Bo Huang, Yuguo Li, Yuanjian Yang, and Meng Gao
Atmos. Chem. Phys., 22, 13341–13353, https://doi.org/10.5194/acp-22-13341-2022, https://doi.org/10.5194/acp-22-13341-2022, 2022
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Unprecedented urbanization in China has led to serious urban heat island (UHI) issues, exerting intense heat stress on urban residents. We find diverse influences of aerosol pollution on urban heat island intensity (UHII) under different circulations. Our results also highlight the role of black carbon in aggravating UHI, especially during nighttime. It could thus be targeted for cooperative management of heat islands and aerosol pollution.
Qianqian Song, Zhibo Zhang, Hongbin Yu, Jasper F. Kok, Claudia Di Biagio, Samuel Albani, Jianyu Zheng, and Jiachen Ding
Atmos. Chem. Phys., 22, 13115–13135, https://doi.org/10.5194/acp-22-13115-2022, https://doi.org/10.5194/acp-22-13115-2022, 2022
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This study developed a dataset that enables us to efficiently calculate dust direct radiative effect (DRE, i.e., cooling or warming our planet) for any given dust size distribution in addition to three sets of dust mineral components and two dust shapes. We demonstrate and validate the method of using this dataset to calculate dust DRE. Moreover, using this dataset we found that dust mineral composition is a more important factor in determining dust DRE than dust size and shape.
Eleni Drakaki, Vassilis Amiridis, Alexandra Tsekeri, Antonis Gkikas, Emmanouil Proestakis, Sotirios Mallios, Stavros Solomos, Christos Spyrou, Eleni Marinou, Claire L. Ryder, Demetri Bouris, and Petros Katsafados
Atmos. Chem. Phys., 22, 12727–12748, https://doi.org/10.5194/acp-22-12727-2022, https://doi.org/10.5194/acp-22-12727-2022, 2022
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State-of-the-art atmospheric dust models have limitations in accounting for a realistic dust size distribution (emission, transport). We modify the parameterization of the mineral dust cycle by including particles with diameter >20 μm, as indicated by observations over deserts. Moreover, we investigate the effects of reduced settling velocities of dust particles. Model results are evaluated using airborne and spaceborne dust measurements above Cabo Verde.
Chenguang Tian, Xu Yue, Jun Zhu, Hong Liao, Yang Yang, Yadong Lei, Xinyi Zhou, Hao Zhou, Yimian Ma, and Yang Cao
Atmos. Chem. Phys., 22, 12353–12366, https://doi.org/10.5194/acp-22-12353-2022, https://doi.org/10.5194/acp-22-12353-2022, 2022
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We quantify the impacts of fire aerosols on climate through direct, indirect, and albedo effects. In atmosphere-only simulations, we find global fire aerosols cause surface cooling and rainfall inhibition over many land regions. These fast atmospheric perturbations further lead to a reduction in regional leaf area index and lightning activities. By considering the feedback of fire aerosols on humidity, lightning, and leaf area index, we predict a slight reduction in fire emissions.
Yanxing Wu, Run Liu, Yanzi Li, Junjie Dong, Zhijiong Huang, Junyu Zheng, and Shaw Chen Liu
Atmos. Chem. Phys., 22, 11945–11955, https://doi.org/10.5194/acp-22-11945-2022, https://doi.org/10.5194/acp-22-11945-2022, 2022
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Multiple linear regression (MLR) analyses often interpret the correlation coefficient (r2) as the contribution of an independent variable to the dependent variable. Since a good correlation does not imply a causal relationship, we propose that r2 should be interpreted as the maximum possible contribution. Moreover, MLR results are sensitive to the length of time analyzed; long-term analysis gives a more accurate assessment because of its additional constraints.
Mengying Li, Shaocai Yu, Xue Chen, Zhen Li, Yibo Zhang, Zhe Song, Weiping Liu, Pengfei Li, Xiaoye Zhang, Meigen Zhang, Yele Sun, Zirui Liu, Caiping Sun, Jingkun Jiang, Shuxiao Wang, Benjamin N. Murphy, Kiran Alapaty, Rohit Mathur, Daniel Rosenfeld, and John H. Seinfeld
Atmos. Chem. Phys., 22, 11845–11866, https://doi.org/10.5194/acp-22-11845-2022, https://doi.org/10.5194/acp-22-11845-2022, 2022
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This study constructed an emission inventory of condensable particulate matter (CPM) in China with a focus on organic aerosols (OAs), based on collected CPM emission information. The results show that OA emissions are enhanced twofold for the years 2014 and 2017 after the inclusion of CPM in the new inventory. Sensitivity cases demonstrated the significant contributions of CPM emissions from stationary combustion and mobile sources to primary, secondary, and total OA concentrations.
Petri Räisänen, Joonas Merikanto, Risto Makkonen, Mikko Savolahti, Alf Kirkevåg, Maria Sand, Øyvind Seland, and Antti-Ilari Partanen
Atmos. Chem. Phys., 22, 11579–11602, https://doi.org/10.5194/acp-22-11579-2022, https://doi.org/10.5194/acp-22-11579-2022, 2022
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A climate model is used to evaluate how the radiative forcing (RF) associated with black carbon (BC) emissions depends on the latitude, longitude, and seasonality of emissions. It is found that both the direct RF (BC absorption of solar radiation in air) and snow RF (BC absorption in snow/ice) depend strongly on the emission region and season. The results suggest that, for a given mass of BC emitted, climatic impacts are likely to be largest for high-latitude emissions due to the large snow RF.
Xipeng Jin, Xuhui Cai, Mingyuan Yu, Yu Song, Xuesong Wang, Hongsheng Zhang, and Tong Zhu
Atmos. Chem. Phys., 22, 11409–11427, https://doi.org/10.5194/acp-22-11409-2022, https://doi.org/10.5194/acp-22-11409-2022, 2022
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Meteorological discontinuities in the vertical direction define the lowest atmosphere as the boundary layer, while in the horizontal direction it identifies the contrast zone as the internal boundary. Both of them determine the polluted air mass dimension over the North China Plain. This study reveals the boundary layer structures under three categories of internal boundaries, modified by thermal, dynamical, and blending effects. It provides a new insight to understand regional pollution.
Lichao Yang, Wansuo Duan, Zifa Wang, and Wenyi Yang
Atmos. Chem. Phys., 22, 11429–11453, https://doi.org/10.5194/acp-22-11429-2022, https://doi.org/10.5194/acp-22-11429-2022, 2022
Short summary
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The initial meteorological state has a great impact on PM2.5 forecasts. Assimilating additional observations is an effective way to improve the accuracy of the initial meteorological state. Here we used an advanced optimization approach to identify where we should preferentially place the meteorological observations associated with PM2.5 forecasts in the Beijing–Tianjin–Hebei region of China. We provide evidence that the target observation strategy is effective for improving PM2.5 forecasts.
Anthony C. Jones, Adrian Hill, John Hemmings, Pascal Lemaitre, Arnaud Quérel, Claire L. Ryder, and Stephanie Woodward
Atmos. Chem. Phys., 22, 11381–11407, https://doi.org/10.5194/acp-22-11381-2022, https://doi.org/10.5194/acp-22-11381-2022, 2022
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As raindrops fall to the ground, they capture aerosol (i.e. below-cloud scavenging or BCS). Many different BCS schemes are available to climate models, and it is unclear what the impact of selecting one scheme over another is. Here, various BCS models are outlined and then applied to mineral dust in climate model simulations. We find that dust concentrations are highly sensitive to the BCS scheme, with dust atmospheric lifetimes ranging from 5 to 44 d.
Zhicong Yin, Mingkeng Duan, Yuyan Li, Tianbao Xu, and Huijun Wang
Atmos. Chem. Phys., 22, 11173–11185, https://doi.org/10.5194/acp-22-11173-2022, https://doi.org/10.5194/acp-22-11173-2022, 2022
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The PM2.5 concentration has been greatly reduced in recent years in China and has entered a crucial stage that required fine seasonal prediction. However, there is still no study aimed at predicting gridded PM2.5 concentration. A model for seasonal prediction of gridded winter PM2.5 concentration in the east of China was developed by analyzing the contributions of emissions and climate variability, which could provide scientific support for air pollution control at the regional and city levels.
Qirui Zhong, Nick Schutgens, Guido van der Werf, Twan van Noije, Kostas Tsigaridis, Susanne E. Bauer, Tero Mielonen, Alf Kirkevåg, Øyvind Seland, Harri Kokkola, Ramiro Checa-Garcia, David Neubauer, Zak Kipling, Hitoshi Matsui, Paul Ginoux, Toshihiko Takemura, Philippe Le Sager, Samuel Rémy, Huisheng Bian, Mian Chin, Kai Zhang, Jialei Zhu, Svetlana G. Tsyro, Gabriele Curci, Anna Protonotariou, Ben Johnson, Joyce E. Penner, Nicolas Bellouin, Ragnhild B. Skeie, and Gunnar Myhre
Atmos. Chem. Phys., 22, 11009–11032, https://doi.org/10.5194/acp-22-11009-2022, https://doi.org/10.5194/acp-22-11009-2022, 2022
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Aerosol optical depth (AOD) errors for biomass burning aerosol (BBA) are evaluated in 18 global models against satellite datasets. Notwithstanding biases in satellite products, they allow model evaluations. We observe large and diverse model biases due to errors in BBA. Further interpretations of AOD diversities suggest large biases exist in key processes for BBA which require better constraining. These results can contribute to further model improvement and development.
Marje Prank, Juha Tonttila, Jaakko Ahola, Harri Kokkola, Thomas Kühn, Sami Romakkaniemi, and Tomi Raatikainen
Atmos. Chem. Phys., 22, 10971–10992, https://doi.org/10.5194/acp-22-10971-2022, https://doi.org/10.5194/acp-22-10971-2022, 2022
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Aerosols and clouds persist as the dominant sources of uncertainty in climate projections. In this modelling study, we investigate the role of marine aerosols in influencing the lifetime of low-level clouds. Our high resolution simulations show that sea spray can both extend and shorten the lifetime of the cloud layer depending on the model setup. The impact of the primary marine organics is relatively limited while secondary aerosol from monoterpenes can have larger impact.
Roger Teoh, Ulrich Schumann, Edward Gryspeerdt, Marc Shapiro, Jarlath Molloy, George Koudis, Christiane Voigt, and Marc E. J. Stettler
Atmos. Chem. Phys., 22, 10919–10935, https://doi.org/10.5194/acp-22-10919-2022, https://doi.org/10.5194/acp-22-10919-2022, 2022
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Aircraft condensation trails (contrails) contribute to over half of the climate forcing attributable to aviation. This study uses historical air traffic and weather data to simulate contrails in the North Atlantic over 5 years, from 2016 to 2021. We found large intra- and inter-year variability in contrail radiative forcing and observed a 66 % reduction due to COVID-19. Most warming contrails predominantly result from night-time flights in winter.
Daniel Peter Grosvenor and Kenneth S. Carslaw
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-583, https://doi.org/10.5194/acp-2022-583, 2022
Revised manuscript accepted for ACP
Short summary
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We determine what causes long-term trends in shortwave radiative fluxes in two climate models. A positive trend occurs between 1850 and 1970 (increasing SW reflection) and a negative trend between 1970 and 2014; the pre-1970 positive trend is mainly driven by an increase in cloud droplet number concentrations due to increases in aerosol and the 1970–2014 trend is driven by a decrease in cloud fraction, which we attribute mainly to changes in clouds caused by greenhouse gas-induced warming.
Haochi Che, Philip Stier, Duncan Watson-Parris, Hamish Gordon, and Lucia Deaconu
Atmos. Chem. Phys., 22, 10789–10807, https://doi.org/10.5194/acp-22-10789-2022, https://doi.org/10.5194/acp-22-10789-2022, 2022
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Extensive stratocumulus clouds over the south-eastern Atlantic (SEA) can lead to a cooling effect on the climate. A key pathway by which aerosols affect cloud properties is by acting as cloud condensation nuclei (CCN). Here, we investigated the source attribution of CCN in the SEA as well as the cloud responses. Our results show that aerosol nucleation contributes most to CCN in the marine boundary layer. In terms of emissions, anthropogenic sources contribute most to the CCN and cloud droplets.
Aditya Kumar, R. Bradley Pierce, Ravan Ahmadov, Gabriel Pereira, Saulo Freitas, Georg Grell, Chris Schmidt, Allen Lenzen, Joshua P. Schwarz, Anne E. Perring, Joseph M. Katich, John Hair, Jose L. Jimenez, Pedro Campuzano-Jost, and Hongyu Guo
Atmos. Chem. Phys., 22, 10195–10219, https://doi.org/10.5194/acp-22-10195-2022, https://doi.org/10.5194/acp-22-10195-2022, 2022
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We use the WRF-Chem model with new implementations of GOES-16 wildfire emissions and plume rise based on fire radiative power (FRP) to interpret aerosol observations during the 2019 NASA–NOAA FIREX-AQ field campaign and perform model evaluations. The model shows significant improvements in simulating the variety of aerosol loading environments sampled during FIREX-AQ. Our results also highlight the importance of accurate wildfire diurnal cycle and aerosol chemical mechanisms in models.
Cited articles
Ayers, G. P., Gillett, R. W., and Gras, J. L.: On the vapor pressure of
sulfuric acid, Geophys. Res. Lett., 7, 433–436,
https://doi.org/10.1029/GL007i006p00433, 1980. a
Ben-Naim, A.: Solvation Thermodynamics, Plenum Press, New York and London,
1987. a
Bondy, A. L., Bonanno, D., Moffet, R. C., Wang, B., Laskin, A., and Ault,
A. P.: The diverse chemical mixing state of aerosol particles in the
southeastern United States, Atmos. Chem. Phys., 18, 12595–12612,
https://doi.org/10.5194/acp-18-12595-2018, 2018. a
Budisulistiorini, S. H., Li, X., Bairai, S. T., Renfro, J., Liu, Y., Liu, Y.,
McKinney, K. A., Martin, S. T., McNeill, V. F., Pye, H. O. T., Nenes, A.,
Neff, M. E., Stone, E. A., Mueller, S., Knote, C., Shaw, S. L., Zhang, Z.,
Gold, A., and Surratt, J. D.: Examining the effects of anthropogenic
emissions on isoprene-derived secondary organic aerosol formation during the
2013 Southern Oxidant and Aerosol Study (SOAS) at the Look Rock, Tennessee
ground site, Atmos. Chem. Phys., 15, 8871–8888,
https://doi.org/10.5194/acp-15-8871-2015, 2015. a
Chan, M. N., Surratt, J. D., Chan, A. W. H., Schilling, K., Offenberg, J. H.,
Lewandowski, M., Edney, E. O., Kleindienst, T. E., Jaoui, M., Edgerton,
E. S., Tanner, R. L., Shaw, S. L., Zheng, M., Knipping, E. M., and Seinfeld,
J. H.: Influence of aerosol acidity on the chemical composition of secondary
organic aerosol from β-caryophyllene, Atmos. Chem. Phys., 11,
1735–1751, https://doi.org/10.5194/acp-11-1735-2011, 2011. a
Clayden, J., Greeves, N., Warren, S., and Wothers, P.: Organic Chemistry,
Oxford University Press, New York, USA, 2001. a
COSMObase: version 17.01, COSMOlogic GmbH & Co. KG.,
Leverkusen, Germany, 2011. a
COSMOconf: version 4.3, COSMOlogic GmbH & Co. KG.,
Leverkusen, Germany, 2013. a
COSMOtherm: version C3.0, Release 18, COSMOlogic GmbH & Co.
KG., Leverkusen, Germany, 2018. a
COSMOtherm: version C3.0, Release 19, COSMOlogic GmbH & Co.
KG., Leverkusen, Germany, 2019. a
D'Ambro, E. L., Schobesberger, S., Gaston, C. J., Lopez-Hilfiker, F. D., Lee,
B. H., Liu, J., Zelenyuk, A., Bell, D., Cappa, C. D., Helgestad, T., Li, Z.,
Guenther, A., Wang, J., Wise, M., Caylor, R., Surratt, J. D., Riedel, T.,
Hyttinen, N., Salo, V.-T., Hasan, G., Kurtén, T., Shilling, J. E., and
Thornton, J. A.: Chamber-based insights into the factors controlling
epoxydiol (IEPOX) secondary organic aerosol (SOA) yield, composition, and
volatility, Atmos. Chem. Phys., 19, 11253–11265,
https://doi.org/10.5194/acp-19-11253-2019, 2019. a
Darer, A. I., Cole-Filipiak, N. C., O'Connor, A. E., and Elrod, M. J.:
Formation and stability of atmospherically relevant isoprene-derived
organosulfates and organonitrates, Environ. Sci. Technol., 45, 1895–1902,
https://doi.org/10.1021/es103797z, 2011. a, b, c
Eckert, F. and Klamt, A.: Fast solvent screening via quantum chemistry:
COSMO-RS approach, AIChE J., 48, 369–385, https://doi.org/10.1002/aic.690480220, 2002. a
Estillore, A. D., Hettiyadura, A. P. S., Qin, Z., Leckrone, E., Wombacher, B.,
Humphry, T., Stone, E. A., and Grassian, V. H.: Water uptake and hygroscopic
growth of organosulfate aerosol, Environ. Sci. Technol., 50, 4259–4268,
https://doi.org/10.1021/acs.est.5b05014, 2016. a, b
Glasius, M., Bering, M. S., Yee, L. D., de Sá, S. S., Isaacman-VanWertz,
G., Wernis, R. A., Barbosa, H. M. J., Alexander, M. L., Palm, B. B., Hu, W.,
Campuzano-Jost, P., Day, D. A., Jimenez, J. L., Shrivastava, M., Martin,
S. T., and Goldstein, A. H.: Organosulfates in aerosols downwind of an urban
region in central Amazon, Environ. Sci.: Process. Impacts, 20, 1546–1558,
https://doi.org/10.1039/C8EM00413G, 2018a. a, b
Glasius, M., Hansen, A. M. K., Claeys, M., Henzing, J. S., Jedynska, A. D.,
Kasper-Giebl, A., Kistler, M., Kristensen, K., Martinsson, J., Maenhaut, W.,
Nøjgaard, J., Spindler, G., Stenström, K. E., Swietlicki, E., Szidat,
S., Simpson, D., and Yttri, K. E.: Composition and sources of carbonaceous
aerosols in Northern Europe during winter, Atmos. Environ., 173, 127–141,
https://doi.org/10.1016/j.atmosenv.2017.11.005, 2018b. a
Halgren, T. A.: Merck molecular force field. I. Basis, form, scope,
parameterization, and performance of MMFF94, J. Comp. Chem., 17, 490–519,
https://doi.org/10.1002/(SICI)1096-987X(199604)17:5/6<490::AID-JCC1>3.0.CO;2-P, 1996. a
Ham, S., Babar, Z. B., Lee, J. B., Lim, H.-J., and Song, M.: Liquid–liquid
phase separation in secondary organic aerosol particles produced from α-pinene ozonolysis and α-pinene photooxidation with/without ammonia,
Atmos. Chem. Phys., 19, 9321–9331, https://doi.org/10.5194/acp-19-9321-2019, 2019. a, b, c
Hansen, A. M. K., Hong, J., Raatikainen, T., Kristensen, K., Ylisirniö, A.,
Virtanen, A., Petäjä, T., Glasius, M., and Prisle, N. L.: Hygroscopic
properties and cloud condensation nuclei activation of limonene-derived
organosulfates and their mixtures with ammonium sulfate, Atmos. Chem. Phys.,
15, 14071–14089, https://doi.org/10.5194/acp-15-14071-2015, 2015. a, b, c, d, e, f, g
Hettiyadura, A. P. S., Jayarathne, T., Baumann, K., Goldstein, A. H., de Gouw,
J. A., Koss, A., Keutsch, F. N., Skog, K., and Stone, E. A.: Qualitative and
quantitative analysis of atmospheric organosulfates in Centreville, Alabama,
Atmos. Chem. Phys., 17, 1343–1359, https://doi.org/10.5194/acp-17-1343-2017, 2017. a
Hettiyadura, A. P. S., Al-Naiema, I. M., Hughes, D. D., Fang, T., and Stone,
E. A.: Organosulfates in Atlanta, Georgia: anthropogenic influences on
biogenic secondary organic aerosol formation, Atmos. Chem. Phys., 19,
3191–3206, https://doi.org/10.5194/acp-19-3191-2019, 2019. a, b
Huang, R.-J., Cao, J., Chen, Y., Yang, L., Shen, J., You, Q., Wang, K., Lin,
C., Xu, W., Gao, B., Li, Y., Chen, Q., Hoffmann, T., O'Dowd, C. D., Bilde,
M., and Glasius, M.: Organosulfates in atmospheric aerosol: synthesis and
quantitative analysis of PM2.5 from Xi'an, northwestern China, Atmos.
Phys. Chem., 11, 3447–3456, https://doi.org/10.5194/amt-11-3447-2018, 2018. a
Hyttinen, N., Elm, J., Malila, J., Calderón, S. M., and Prisle, N. L.:
Supplementary data for the manuscript “Thermodynamic properties of isoprene
and monoterpene derived organosulfates estimated with COSMOtherm”
[Dataset], Zenodo, https://doi.org/10.5281/zenodo.3552309, 2019. a
Iinuma, Y., Böge, O., Kahnt, A., and Herrmann, H.: Laboratory chamber
studies on the formation of organosulfates from reactive uptake of
monoterpene oxides, Phys. Chem. Chem. Phys., 11, 7985–7997,
https://doi.org/10.1039/B904025K, 2009. a, b, c
Klamt, A.: Conductor-like screening model for real solvents: a new approach to
the quantitative calculation of solvation phenomena, J. Phys. Chem., 99,
2224–2235, https://doi.org/10.1021/j100007a062, 1995. a
Klamt, A., Jonas, V., Bürger, T., and Lohrenz, J. C. W.: Refinement and
parametrization of COSMO-RS, J. Phys. Chem. A, 102, 5074–5085,
https://doi.org/10.1021/jp980017s, 1998. a
Klamt, A., Eckert, F., Reinisch, J., and Wichmann, K.: Prediction of
cyclohexane-water distribution coefficients with COSMO-RS on the SAMPL5 data
set, J. Comput.-Aided Mol. Des., 30, 959–967,
https://doi.org/10.1007/s10822-016-9927-y, 2016. a
Kulmala, M. and Laaksonen, A.: Binary nucleation of water–sulfuric acid
system: Comparison of classical theories with different H2SO4
saturation vapor pressures, J. Chem. Phys., 93, 696–701,
https://doi.org/10.1063/1.459519, 1990. a
Kurtén, T., Tiusanen, K., Roldin, P., Rissanen, M., Luy, J.-N., Boy, M.,
Ehn, M., and Donahue, N.: α-Pinene Autoxidation Products May Not Have
Extremely Low Saturation Vapor Pressures Despite High O:C Ratios, J. Phys.
Chem. A, 120, 2569–2582, https://doi.org/10.1021/acs.jpca.6b02196, 2016. a, b, c, d
Le Breton, M., Wang, Y., Hallquist, Å. M., Pathak, R. K., Zheng, J., Yang,
Y., Shang, D., Glasius, M., Bannan, T. J., Liu, Q., Chan, C. K., Percival,
C. J., Zhu, W., Lou, S., Topping, D., Wang, Y., Yu, J., Lu, K., Guo, S., Hu,
M., and Hallquist, M.: Online gas- and particle-phase measurements of
organosulfates, organosulfonates and nitrooxy organosulfates in Beijing
utilizing a FIGAERO ToF-CIMS, Atmos. Phys. Chem., 10, 10355–10371,
https://doi.org/10.5194/acp-18-10355-2018, 2018. a, b
Liggio, J. and Li, S.-M.: Organosulfate formation during the uptake of
pinonaldehyde on acidic sulfate aerosols, Geophys. Res. Lett., 33, L13808,
https://doi.org/10.1029/2006GL026079, 2006. a
Minerath, E. C. and Elrod, M. J.: Assessing the potential for diol and hydroxy
sulfate ester formation from the reaction of epoxides in tropospheric
aerosols, Environ. Sci. Technol., 43, 1386–1392, https://doi.org/10.1021/es8029076,
2009. a
Nguyen, Q., Christensen, M. K., Cozzi, F., Zare, A., Hansen, A. M. K.,
Kristensen, K., Tulinius, T. E., Madsen, H. H., Christensen, J. H., Brandt,
J., Massling, A., Nøjgaard, J. K., and Glasius, M.: Understanding the
anthropogenic influence on formation of biogenic secondary organic aerosols
in Denmark via analysis of organosulfates and related oxidation products,
Atmos. Chem. Phys., 14, 8961–8981, https://doi.org/10.5194/acp-14-8961-2014,
2014a. a
Nguyen, Q. T., Kristensen, T. B., Hansen, A. M. K., Skov, H., Bossi, R.,
Massling, A., Sørensen, L. L., Bilde, M., Glasius, M., and Nøjgaard,
J. K.: Characterization of humic-like substances in Arctic aerosols, J.
Geophys. Res.-Atmos., 119, 5011–5027, https://doi.org/10.1002/2013JD020144,
2014b. a
Noppel, M., Vehkamäki, H., and Kulmala, M.: An improved model for hydrate
formation in sulfuric acid–water nucleation, J. Chem. Phys., 116, 218–228,
https://doi.org/10.1063/1.1423333, 2002. a
Prigogine, I. and Defay, R.: Chemical Thermodynamics, Longmans Green, London,
1st edn., 1954. a
Prisle, N. L., Engelhart, G. J., Bilde, M., and Donahue, N. M.: Humidity
influence on gas-particle phase partitioning of α-pinene + O3
secondary organic aerosol, Geophys. Res. Lett., 37, L01802,
https://doi.org/10.1029/2009GL041402, 2010. a
Rastak, N., Pajunoja, A., Acosta Navarro, J. C., Ma, J., Song, M., Partridge,
D. G., Kirkevåg, A., Leong, Y., Hu, W., Taylor, N. F., Lambe, A.,
Cerully, K., Bougiatioti, A., Liu, P., Krejci, R., Petäjä, T.,
Percival, C., Davidovits, P., Worsnop, D. R., Ekman, A. M. L., Nenes, A.,
Martin, S., Jimenez, J. L., Collins, D. R., Topping, D. O., Bertram, A. K.,
Zuend, A., Virtanen, A., and Riipinen, I.: Microphysical explanation of the
RH-dependent water affinity of biogenic organic aerosol and its importance
for climate, Geophys. Res. Lett., 44, 5167–5177, https://doi.org/10.1002/2017GL073056,
2017. a, b
Schindelka, J., Iinuma, Y., Hoffmann, D., and Herrmann, H.: Sulfate
radical-initiated formation of isoprene-derived organosulfates in atmospheric
aerosols, Faraday Discuss., 165, 237–259, https://doi.org/10.1039/C3FD00042G, 2013. a
Schröder, B., Fulem, M., and Martins, M. A. R.: Vapor pressure predictions
of multi-functional oxygen-containing organic compounds with COSMO-RS, Atmos.
Environ., 133, 135–144, https://doi.org/10.1016/j.atmosenv.2016.03.036, 2016. a
Shinoda, K., Hiruta, S., and Amaya, K.: The heat of solution and of wetting of
ionic surfactants close to the Krafft points, J. Colloid Interface Sci., 21,
102–106, https://doi.org/10.1016/0095-8522(66)90085-7, 1966. a, b
Song, M., Marcolli, C., Krieger, U. K., Zuend, A., and Peter, T.:
Liquid–liquid phase separation in aerosol particles: Dependence on O:C,
organic functionalities, and compositional complexity, Geophys. Res. Lett.,
39, L19801, https://doi.org/10.1029/2012GL052807, 2012. a, b, c
Song, M., Ham, S., Andrews, R. J., You, Y., and Bertram, A. K.: Liquid–liquid
phase separation in organic particles containing one and two organic species:
importance of the average O : C, Atmos. Chem. Phys., 18, 12075–12084,
https://doi.org/10.5194/acp-18-12075-2018, 2018. a, b, c
Surratt, J. D., Kroll, J. H., Kleindienst, T. E., Edney, E. O., Claeys, M.,
Sorooshian, A., Ng, N. L., Offenberg, J. H., Lewandowski, M., Jaoui, M.,
Flagan, R. C., and Seinfeld, J. H.: Evidence for organosulfates in secondary
organic aerosol, Environ. Sci. Technol., 41, 517–527,
https://doi.org/10.1021/es062081q, 2007. a, b, c, d
Surratt, J. D., Gómez-González, Y., Chan, A. W., Vermeylen, R.,
Shahgholi, M., Kleindienst, T. E., Edney, E. O., Offenberg, J. H.,
Lewandowski, M., Jaoui, M., Maenhaut, W., Claeys, M., Flagan, R. C., and
Seinfeld, J. H.: Organosulfate formation in biogenic secondary organic
aerosol, J. Phys. Chem. A, 112, 8345–8378, https://doi.org/10.1021/jp802310p, 2008. a, b, c
Surratt, J. D., Chan, A. W., Eddingsaas, N. C., Chan, M., Loza, C. L., Kwan,
A. J., Hersey, S. P., Flagan, R. C., Wennberg, P. O., and Seinfeld, J. H.:
Reactive intermediates revealed in secondary organic aerosol formation from
isoprene, P. Natl. Acad. Sci. USA, 107, 6640–6645,
https://doi.org/10.1073/pnas.0911114107, 2010. a, b
Tang, I. N. and Munkelwitz, H. R.: Water activities, densities, and refractive
indices of aqueous sulfates and sodium nitrate droplets of atmospheric
importance, J. Geophys. Res.-Atmos., 99, 18801–18808,
https://doi.org/10.1029/94JD01345, 1994. a, b, c, d
Toivola, M., Prisle, N. L., Elm, J., Waxman, E. M., Volkamer, R., and
Kurtén, T.: Can COSMOTherm Predict a Salting in Effect?, J. Phys. Chem.
A, 121, 6288–6295, https://doi.org/10.1021/acs.jpca.7b04847, 2017. a
Toure, O., Audonnet, F., Lebert, A., and Dussap, C.-G.: COSMO-RS-PDHS: a new
predictive model for aqueous electrolytes solutions, Chem. Eng. Res. Des.,
92, 2873–2883, https://doi.org/10.1016/j.cherd.2014.06.020, 2014. a, b
TURBOMOLE: Version 7.11, a development of University of Karlsruhe and
Forschungszentrum Karlsruhe GmbH, TURBOMOLE GmbH, 2010. a
Wach, P., Spólnik, G., Rudziński, K. J., Skotak, K., Claeys, M.,
Danikiewicz, W., and Szmigielski, R.: Radical oxidation of methyl vinyl
ketone and methacrolein in aqueous droplets: Characterization of
organosulfates and atmospheric implications, Chemosphere, 214, 1–9,
https://doi.org/10.1016/j.chemosphere.2018.09.026, 2019. a
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. a, b, c, d
Wang, C., Lei, Y. D., and Wania, F.: Effect of Sodium Sulfate, Ammonium
Chloride, Ammonium Nitrate, and Salt Mixtures on Aqueous Phase Partitioning
of Organic Compounds, Environ. Sci. Technol., 50, 12742–12749,
https://doi.org/10.1021/acs.est.6b03525, 2016. a
Wavefunction Inc.: Spartan'14, Irvine, CA, 2014. a
Woods III, E., Kim, H. S., Wivagg, C. N., Dotson, S. J., Broekhuizen, K. E.,
and Frohardt, E. F.: Phase transitions and surface morphology of
surfactant-coated aerosol particles, J. Phys. Chem. A, 111, 11013–11020,
https://doi.org/10.1021/jp074848m, 2007. a
Wu, F.-M., Wang, X.-W., Jing, B., Zhang, Y.-H., and Ge, M.-F.: Liquid–liquid
phase separation in internally mixed magnesium sulfate/glutaric acid
particles, Atmos. Environ., 178, 286–292,
https://doi.org/10.1016/j.atmosenv.2018.02.012, 2018. a
Xu, L., Guo, H., Boyd, C. M., Klein, M., Bougiatioti, A., Cerully, K. M., Hite,
J. R., Isaacman-VanWertz, G., Kreisberg, N. M., Knote, C., Olson, K., Koss,
A., Goldstein, A. H., Hering, S. V., de Gouw, J., Baumann, K., Lee, S.-H.,
Nenes, A., Weber, R. J., and Ng, N. L.: Effects of anthropogenic emissions on
aerosol formation from isoprene and monoterpenes in the southeastern United
States, P. Natl. Acad. Sci. USA, 112, 37–42, https://doi.org/10.1073/pnas.1417609112,
2015.
a
Zhang, Y., Chen, Y., Lambe, A. T., Olson, N. E., Lei, Z., Craig, R. L., Zhang,
Z., Gold, A., Onasch, T. B., Jayne, J. T., Worsnop, D. R., Gaston, C. J.,
Thornton, J. A., Vizuete, W., Ault, A. P., and Surratt, J. D.: Effect of the
aerosol-phase state on secondary organic aerosol formation from the reactive
uptake of isoprene-derived epoxydiols (IEPOX), Environ. Sci. Technol. Lett.,
5, 167–174, https://doi.org/10.1021/acs.estlett.8b00044, 2018. a
Short summary
Organosulfates have been identified in atmospheric secondary organic aerosol (SOA). The thermodynamic properties of SOA constituents, such as organosulfates, affect the stability and atmospheric impact of the SOA. Here we present estimated solubility, activity, pKa, saturation vapor pressure and Henry's law solubility values for several atmospherically relevant monoterpene- and isoprene-derived organosulfate compounds. These properties can be used, for example, in aerosol process modeling.
Organosulfates have been identified in atmospheric secondary organic aerosol (SOA). The...
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