Measurement report: Distinct size dependence and diurnal variation in organic aerosol hygroscopicity, volatility, and cloud condensation nuclei activity at a rural site in the Pearl River Delta (PRD) region, China

<p>Organic aerosol (OA) has a significant contribution to cloud formation and hence climate change. However, high uncertainties still exist in its impact on global climate, owing to the varying physical properties affected by the complex formation and aging processes. In this study, the hygros...

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Main Authors: M. Cai, S. Huang, B. Liang, Q. Sun, L. Liu, B. Yuan, M. Shao, W. Hu, W. Chen, Q. Song, W. Li, Y. Peng, Z. Wang, D. Chen, H. Tan, H. Xu, F. Li, X. Deng, T. Deng, J. Sun, J. Zhao
Format: Article
Language:English
Published: Copernicus Publications 2022-06-01
Series:Atmospheric Chemistry and Physics
Online Access:https://acp.copernicus.org/articles/22/8117/2022/acp-22-8117-2022.pdf
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author M. Cai
M. Cai
S. Huang
B. Liang
Q. Sun
L. Liu
B. Yuan
M. Shao
W. Hu
W. Chen
Q. Song
W. Li
Y. Peng
Z. Wang
D. Chen
H. Tan
H. Xu
F. Li
F. Li
X. Deng
T. Deng
J. Sun
J. Zhao
J. Zhao
J. Zhao
author_facet M. Cai
M. Cai
S. Huang
B. Liang
Q. Sun
L. Liu
B. Yuan
M. Shao
W. Hu
W. Chen
Q. Song
W. Li
Y. Peng
Z. Wang
D. Chen
H. Tan
H. Xu
F. Li
F. Li
X. Deng
T. Deng
J. Sun
J. Zhao
J. Zhao
J. Zhao
author_sort M. Cai
collection DOAJ
description <p>Organic aerosol (OA) has a significant contribution to cloud formation and hence climate change. However, high uncertainties still exist in its impact on global climate, owing to the varying physical properties affected by the complex formation and aging processes. In this study, the hygroscopicity, volatility, cloud condensation nuclei (CCN) activity, and chemical composition of particles were measured using a series of online instruments at a rural site in the Pearl River Delta (PRD) region of China in fall 2019. During the campaign, the average hygroscopicity of OA (<span class="inline-formula"><i>κ</i><sub>OA</sub></span>) increased from 0.058 at 30 <span class="inline-formula">nm</span> to 0.09 at 200 <span class="inline-formula">nm</span>, suggesting a higher oxidation state of OA at larger particle sizes, supported by a higher fraction of extremely low volatility OA (ELVOA) for larger size particles. Significantly different diurnal patterns of <span class="inline-formula"><i>κ</i><sub>OA</sub></span> were observed between Aitken mode particles and accumulation mode particles. For Aitken mode particles (30–100 <span class="inline-formula">nm</span>), the <span class="inline-formula"><i>κ</i><sub>OA</sub></span> values showed daily minima (0.02–0.07) during daytime, while the accumulation mode exhibited a daytime peak (<span class="inline-formula">∼</span> 0.09). Coincidently, a daytime peak was observed for both aged biomass burning organic aerosol (aBBOA) and less oxygenated organic aerosol (LOOA) based on source apportionment, which was attributed to the aging processes and gas–particle partitioning through photochemical reactions. In addition, the fraction of semi-volatile OA (SVOA) was higher at all measured sizes during daytime than during nighttime. These results indicate that the formation of secondary OA (SOA) through gas–particle partitioning can generally occur at all diameters, while the aging processes of pre-existing particles are more dominated in the accumulation mode. Furthermore, we found that applying a fixed <span class="inline-formula"><i>κ</i><sub>OA</sub></span> value (0.1) could lead to an overestimation of the CCN number concentration (<span class="inline-formula"><i>N</i><sub>CCN</sub></span>) up to 12 %–19 % at 0.1 %–0.7 % supersaturation (SS), which was more obvious at higher SS during daytime. Better prediction of <span class="inline-formula"><i>N</i><sub>CCN</sub></span> could be achieved by using size-resolved diurnal <span class="inline-formula"><i>κ</i><sub>OA</sub></span>, which indicates that the size dependence and diurnal variations in <span class="inline-formula"><i>κ</i><sub>OA</sub></span> can strongly affect the <span class="inline-formula"><i>N</i><sub>CCN</sub></span> at different SS values. Our results highlight the need for accurately evaluating the atmospheric evolution of OA at different size ranges and their impact on the physicochemical properties and hence climate effects.</p>
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spelling doaj.art-3aa2a5de3fb54c1785722dc31c0a29ee2022-12-22T00:20:06ZengCopernicus PublicationsAtmospheric Chemistry and Physics1680-73161680-73242022-06-01228117813610.5194/acp-22-8117-2022Measurement report: Distinct size dependence and diurnal variation in organic aerosol hygroscopicity, volatility, and cloud condensation nuclei activity at a rural site in the Pearl River Delta (PRD) region, ChinaM. Cai0M. Cai1S. Huang2B. Liang3Q. Sun4L. Liu5B. Yuan6M. Shao7W. Hu8W. Chen9Q. Song10W. Li11Y. Peng12Z. Wang13D. Chen14H. Tan15H. Xu16F. Li17F. Li18X. Deng19T. Deng20J. Sun21J. Zhao22J. Zhao23J. Zhao24Institute for Environmental and Climate Research, Jinan University, Guangdong-Hongkong-Macau Joint Laboratory of Collaborative Innovation for Environmental Quality, Guangzhou, 511443, ChinaGuangdong Province Engineering Laboratory for Air Pollution Control, Guangdong Provincial Key Laboratory of Water and Air Pollution Control, South China Institute of Environmental Sciences, MEE, Guangzhou 510655, ChinaInstitute for Environmental and Climate Research, Jinan University, Guangdong-Hongkong-Macau Joint Laboratory of Collaborative Innovation for Environmental Quality, Guangzhou, 511443, ChinaSchool of Atmospheric Sciences, Guangdong Province Key Laboratory for Climate Change and Natural Disaster Studies, and Institute of Earth Climate and Environment System, Sun Yat-sen University, Zhuhai, Guangdong 519082, ChinaSchool of Atmospheric Sciences, Guangdong Province Key Laboratory for Climate Change and Natural Disaster Studies, and Institute of Earth Climate and Environment System, Sun Yat-sen University, Zhuhai, Guangdong 519082, ChinaInstitute of Tropical and Marine Meteorology of China Meteorological Administration, Guangzhou 510640, ChinaInstitute for Environmental and Climate Research, Jinan University, Guangdong-Hongkong-Macau Joint Laboratory of Collaborative Innovation for Environmental Quality, Guangzhou, 511443, ChinaInstitute for Environmental and Climate Research, Jinan University, Guangdong-Hongkong-Macau Joint Laboratory of Collaborative Innovation for Environmental Quality, Guangzhou, 511443, ChinaState Key Laboratory of Organic Geochemistry and Guangdong Key Laboratory of Environmental Protection and Resources Utilization, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, ChinaGuangdong Environmental Monitoring Center, Guangzhou 510308, ChinaInstitute for Environmental and Climate Research, Jinan University, Guangdong-Hongkong-Macau Joint Laboratory of Collaborative Innovation for Environmental Quality, Guangzhou, 511443, ChinaInstitute for Environmental and Climate Research, Jinan University, Guangdong-Hongkong-Macau Joint Laboratory of Collaborative Innovation for Environmental Quality, Guangzhou, 511443, ChinaInstitute for Environmental and Climate Research, Jinan University, Guangdong-Hongkong-Macau Joint Laboratory of Collaborative Innovation for Environmental Quality, Guangzhou, 511443, ChinaInstitute for Environmental and Climate Research, Jinan University, Guangdong-Hongkong-Macau Joint Laboratory of Collaborative Innovation for Environmental Quality, Guangzhou, 511443, ChinaGuangdong Environmental Monitoring Center, Guangzhou 510308, ChinaInstitute of Tropical and Marine Meteorology of China Meteorological Administration, Guangzhou 510640, ChinaSchool of Atmospheric Sciences, Guangdong Province Key Laboratory for Climate Change and Natural Disaster Studies, and Institute of Earth Climate and Environment System, Sun Yat-sen University, Zhuhai, Guangdong 519082, ChinaInstitute of Tropical and Marine Meteorology of China Meteorological Administration, Guangzhou 510640, ChinaXiamen Key Laboratory of Straits Meteorology, Xiamen Meteorological Bureau, Xiamen 361012, ChinaInstitute of Tropical and Marine Meteorology of China Meteorological Administration, Guangzhou 510640, ChinaInstitute of Tropical and Marine Meteorology of China Meteorological Administration, Guangzhou 510640, ChinaGuangdong Province Engineering Laboratory for Air Pollution Control, Guangdong Provincial Key Laboratory of Water and Air Pollution Control, South China Institute of Environmental Sciences, MEE, Guangzhou 510655, ChinaInstitute of Tropical and Marine Meteorology of China Meteorological Administration, Guangzhou 510640, ChinaSouthern Marine Science and Engineering Guangdong Laboratory (Zhuhai), Zhuhai, Guangdong 519082, ChinaGuangdong Provincial Observation and Research Station for Climate Environment and Air Quality Change in the Pearl River Estuary, Guangzhou, Guangdong 510275, China<p>Organic aerosol (OA) has a significant contribution to cloud formation and hence climate change. However, high uncertainties still exist in its impact on global climate, owing to the varying physical properties affected by the complex formation and aging processes. In this study, the hygroscopicity, volatility, cloud condensation nuclei (CCN) activity, and chemical composition of particles were measured using a series of online instruments at a rural site in the Pearl River Delta (PRD) region of China in fall 2019. During the campaign, the average hygroscopicity of OA (<span class="inline-formula"><i>κ</i><sub>OA</sub></span>) increased from 0.058 at 30 <span class="inline-formula">nm</span> to 0.09 at 200 <span class="inline-formula">nm</span>, suggesting a higher oxidation state of OA at larger particle sizes, supported by a higher fraction of extremely low volatility OA (ELVOA) for larger size particles. Significantly different diurnal patterns of <span class="inline-formula"><i>κ</i><sub>OA</sub></span> were observed between Aitken mode particles and accumulation mode particles. For Aitken mode particles (30–100 <span class="inline-formula">nm</span>), the <span class="inline-formula"><i>κ</i><sub>OA</sub></span> values showed daily minima (0.02–0.07) during daytime, while the accumulation mode exhibited a daytime peak (<span class="inline-formula">∼</span> 0.09). Coincidently, a daytime peak was observed for both aged biomass burning organic aerosol (aBBOA) and less oxygenated organic aerosol (LOOA) based on source apportionment, which was attributed to the aging processes and gas–particle partitioning through photochemical reactions. In addition, the fraction of semi-volatile OA (SVOA) was higher at all measured sizes during daytime than during nighttime. These results indicate that the formation of secondary OA (SOA) through gas–particle partitioning can generally occur at all diameters, while the aging processes of pre-existing particles are more dominated in the accumulation mode. Furthermore, we found that applying a fixed <span class="inline-formula"><i>κ</i><sub>OA</sub></span> value (0.1) could lead to an overestimation of the CCN number concentration (<span class="inline-formula"><i>N</i><sub>CCN</sub></span>) up to 12 %–19 % at 0.1 %–0.7 % supersaturation (SS), which was more obvious at higher SS during daytime. Better prediction of <span class="inline-formula"><i>N</i><sub>CCN</sub></span> could be achieved by using size-resolved diurnal <span class="inline-formula"><i>κ</i><sub>OA</sub></span>, which indicates that the size dependence and diurnal variations in <span class="inline-formula"><i>κ</i><sub>OA</sub></span> can strongly affect the <span class="inline-formula"><i>N</i><sub>CCN</sub></span> at different SS values. Our results highlight the need for accurately evaluating the atmospheric evolution of OA at different size ranges and their impact on the physicochemical properties and hence climate effects.</p>https://acp.copernicus.org/articles/22/8117/2022/acp-22-8117-2022.pdf
spellingShingle M. Cai
M. Cai
S. Huang
B. Liang
Q. Sun
L. Liu
B. Yuan
M. Shao
W. Hu
W. Chen
Q. Song
W. Li
Y. Peng
Z. Wang
D. Chen
H. Tan
H. Xu
F. Li
F. Li
X. Deng
T. Deng
J. Sun
J. Zhao
J. Zhao
J. Zhao
Measurement report: Distinct size dependence and diurnal variation in organic aerosol hygroscopicity, volatility, and cloud condensation nuclei activity at a rural site in the Pearl River Delta (PRD) region, China
Atmospheric Chemistry and Physics
title Measurement report: Distinct size dependence and diurnal variation in organic aerosol hygroscopicity, volatility, and cloud condensation nuclei activity at a rural site in the Pearl River Delta (PRD) region, China
title_full Measurement report: Distinct size dependence and diurnal variation in organic aerosol hygroscopicity, volatility, and cloud condensation nuclei activity at a rural site in the Pearl River Delta (PRD) region, China
title_fullStr Measurement report: Distinct size dependence and diurnal variation in organic aerosol hygroscopicity, volatility, and cloud condensation nuclei activity at a rural site in the Pearl River Delta (PRD) region, China
title_full_unstemmed Measurement report: Distinct size dependence and diurnal variation in organic aerosol hygroscopicity, volatility, and cloud condensation nuclei activity at a rural site in the Pearl River Delta (PRD) region, China
title_short Measurement report: Distinct size dependence and diurnal variation in organic aerosol hygroscopicity, volatility, and cloud condensation nuclei activity at a rural site in the Pearl River Delta (PRD) region, China
title_sort measurement report distinct size dependence and diurnal variation in organic aerosol hygroscopicity volatility and cloud condensation nuclei activity at a rural site in the pearl river delta prd region china
url https://acp.copernicus.org/articles/22/8117/2022/acp-22-8117-2022.pdf
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