Using different assumptions of aerosol mixing state and chemical composition to predict CCN concentrations based on field measurements in urban Beijing

Understanding the impacts of aerosol chemical composition and mixing state on cloud condensation nuclei (CCN) activity in polluted areas is crucial for accurately predicting CCN number concentrations (<i>N</i><sub>CCN</sub>). In this study, we predict <i>N</i>&...

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Main Authors: J. Ren, F. Zhang, Y. Wang, D. Collins, X. Fan, X. Jin, W. Xu, Y. Sun, M. Cribb, Z. Li
Format: Article
Language:English
Published: Copernicus Publications 2018-05-01
Series:Atmospheric Chemistry and Physics
Online Access:https://www.atmos-chem-phys.net/18/6907/2018/acp-18-6907-2018.pdf
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author J. Ren
F. Zhang
F. Zhang
Y. Wang
D. Collins
X. Fan
X. Jin
W. Xu
W. Xu
Y. Sun
Y. Sun
M. Cribb
Z. Li
Z. Li
author_facet J. Ren
F. Zhang
F. Zhang
Y. Wang
D. Collins
X. Fan
X. Jin
W. Xu
W. Xu
Y. Sun
Y. Sun
M. Cribb
Z. Li
Z. Li
author_sort J. Ren
collection DOAJ
description Understanding the impacts of aerosol chemical composition and mixing state on cloud condensation nuclei (CCN) activity in polluted areas is crucial for accurately predicting CCN number concentrations (<i>N</i><sub>CCN</sub>). In this study, we predict <i>N</i><sub>CCN</sub> under five assumed schemes of aerosol chemical composition and mixing state based on field measurements in Beijing during the winter of 2016. Our results show that the best closure is achieved with the assumption of size dependent chemical composition for which sulfate, nitrate, secondary organic aerosols, and aged black carbon are internally mixed with each other but externally mixed with primary organic aerosol and fresh black carbon (external–internal size-resolved, abbreviated as EI–SR scheme). The resulting ratios of predicted-to-measured <i>N</i><sub>CCN</sub> (<i>R</i><sub>CCN_p∕m</sub>) were 0.90 – 0.98 under both clean and polluted conditions. Assumption of an internal mixture and bulk chemical composition (INT–BK scheme) shows good closure with <i>R</i><sub>CCN_p∕m</sub> of 1.0 –1.16 under clean conditions, implying that it is adequate for CCN prediction in continental clean regions. On polluted days, assuming the aerosol is internally mixed and has a chemical composition that is size dependent (INT–SR scheme) achieves better closure than the INT–BK scheme due to the heterogeneity and variation in particle composition at different sizes. The improved closure achieved using the EI–SR and INT–SR assumptions highlight the importance of measuring size-resolved chemical composition for CCN predictions in polluted regions. <i>N</i><sub>CCN</sub> is significantly underestimated (with <i>R</i><sub>CCN_p∕m</sub> of 0.66 – 0.75) when using the schemes of external mixtures with bulk (EXT–BK scheme) or size-resolved composition (EXT–SR scheme), implying that primary particles experience rapid aging and physical mixing processes in urban Beijing. However, our results show that the aerosol mixing state plays a minor role in CCN prediction when the <i>κ</i><sub>org</sub> exceeds 0.1.
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spelling doaj.art-d37035fe07f54fcca79236681129bdb32022-12-22T01:22:26ZengCopernicus PublicationsAtmospheric Chemistry and Physics1680-73161680-73242018-05-01186907692110.5194/acp-18-6907-2018Using different assumptions of aerosol mixing state and chemical composition to predict CCN concentrations based on field measurements in urban BeijingJ. Ren0F. Zhang1F. Zhang2Y. Wang3D. Collins4X. Fan5X. Jin6W. Xu7W. Xu8Y. Sun9Y. Sun10M. Cribb11Z. Li12Z. Li13College of Global Change and Earth System Science, Beijing Normal University, Beijing 100875, ChinaCollege of Global Change and Earth System Science, Beijing Normal University, Beijing 100875, ChinaJoint Center for Global Change Studies (JCGCS), Beijing 100875, ChinaCollege of Global Change and Earth System Science, Beijing Normal University, Beijing 100875, ChinaDepartment of Atmospheric Sciences, Texas A & M University, College Station, TX, USACollege of Global Change and Earth System Science, Beijing Normal University, Beijing 100875, ChinaCollege of Global Change and Earth System Science, Beijing Normal University, Beijing 100875, ChinaState Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, ChinaUniversity of Chinese Academy of Sciences, Beijing 100049, ChinaState Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, ChinaUniversity of Chinese Academy of Sciences, Beijing 100049, ChinaEarth System Science Interdisciplinary Center and Department of Atmospheric and Oceanic Science, University of Maryland, College Park, MD, USACollege of Global Change and Earth System Science, Beijing Normal University, Beijing 100875, ChinaEarth System Science Interdisciplinary Center and Department of Atmospheric and Oceanic Science, University of Maryland, College Park, MD, USAUnderstanding the impacts of aerosol chemical composition and mixing state on cloud condensation nuclei (CCN) activity in polluted areas is crucial for accurately predicting CCN number concentrations (<i>N</i><sub>CCN</sub>). In this study, we predict <i>N</i><sub>CCN</sub> under five assumed schemes of aerosol chemical composition and mixing state based on field measurements in Beijing during the winter of 2016. Our results show that the best closure is achieved with the assumption of size dependent chemical composition for which sulfate, nitrate, secondary organic aerosols, and aged black carbon are internally mixed with each other but externally mixed with primary organic aerosol and fresh black carbon (external–internal size-resolved, abbreviated as EI–SR scheme). The resulting ratios of predicted-to-measured <i>N</i><sub>CCN</sub> (<i>R</i><sub>CCN_p∕m</sub>) were 0.90 – 0.98 under both clean and polluted conditions. Assumption of an internal mixture and bulk chemical composition (INT–BK scheme) shows good closure with <i>R</i><sub>CCN_p∕m</sub> of 1.0 –1.16 under clean conditions, implying that it is adequate for CCN prediction in continental clean regions. On polluted days, assuming the aerosol is internally mixed and has a chemical composition that is size dependent (INT–SR scheme) achieves better closure than the INT–BK scheme due to the heterogeneity and variation in particle composition at different sizes. The improved closure achieved using the EI–SR and INT–SR assumptions highlight the importance of measuring size-resolved chemical composition for CCN predictions in polluted regions. <i>N</i><sub>CCN</sub> is significantly underestimated (with <i>R</i><sub>CCN_p∕m</sub> of 0.66 – 0.75) when using the schemes of external mixtures with bulk (EXT–BK scheme) or size-resolved composition (EXT–SR scheme), implying that primary particles experience rapid aging and physical mixing processes in urban Beijing. However, our results show that the aerosol mixing state plays a minor role in CCN prediction when the <i>κ</i><sub>org</sub> exceeds 0.1.https://www.atmos-chem-phys.net/18/6907/2018/acp-18-6907-2018.pdf
spellingShingle J. Ren
F. Zhang
F. Zhang
Y. Wang
D. Collins
X. Fan
X. Jin
W. Xu
W. Xu
Y. Sun
Y. Sun
M. Cribb
Z. Li
Z. Li
Using different assumptions of aerosol mixing state and chemical composition to predict CCN concentrations based on field measurements in urban Beijing
Atmospheric Chemistry and Physics
title Using different assumptions of aerosol mixing state and chemical composition to predict CCN concentrations based on field measurements in urban Beijing
title_full Using different assumptions of aerosol mixing state and chemical composition to predict CCN concentrations based on field measurements in urban Beijing
title_fullStr Using different assumptions of aerosol mixing state and chemical composition to predict CCN concentrations based on field measurements in urban Beijing
title_full_unstemmed Using different assumptions of aerosol mixing state and chemical composition to predict CCN concentrations based on field measurements in urban Beijing
title_short Using different assumptions of aerosol mixing state and chemical composition to predict CCN concentrations based on field measurements in urban Beijing
title_sort using different assumptions of aerosol mixing state and chemical composition to predict ccn concentrations based on field measurements in urban beijing
url https://www.atmos-chem-phys.net/18/6907/2018/acp-18-6907-2018.pdf
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