21 Jan 2022
21 Jan 2022
Status: a revised version of this preprint is currently under review for the journal ACP.

Measurement Report: Distinct size dependence and diurnal variation of OA hygroscopicity, volatility, and CCN activity at a rural site in the Pearl River Delta (PRD) region, China

Mingfu Cai1,2,3, Shan Huang1,2, Baoling Liang4, Qibin Sun4, Li Liu5, Bin Yuan1,2, Min Shao1,2, Weiwei Hu6, Wei Chen6, Qicong Song1,2, Wei Li1,2, Yuwen Peng1,2, Zelong Wang1,2, Duohong Chen7, Haobo Tan5, Hanbin Xu4, Fei Li5, Xuejiao Deng5, Tao Deng5, Jiaren Sun3, and Jun Zhao4,8,9 Mingfu Cai et al.
  • 1Institute for Environmental and Climate Research, Jinan University, Guangzhou, Guangdong 511443, China
  • 2Guangdong-Hongkong-Macau Joint Laboratory of Collaborative Innovation for Environmental Quality, Guangzhou, Guangdong 511443, China
  • 3Guangdong 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, Guangdong 510655, China
  • 4School 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, China
  • 5Institute of Tropical and Marine Meteorology of China Meteorological Administration, Guangzhou 510640, China
  • 6State 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, China
  • 7Guangdong Environmental Monitoring Center, Guangzhou 510308, China
  • 8Southern Marine Science and Engineering Guangdong Laboratory (Zhuhai), Zhuhai, Guangdong 519082, China
  • 9Guangdong Provincial Observation and Research Station for Climate Environment and Air Quality Change in the Pearl River Estuary, Guangzhou, Guangdong 510275, China

Abstract. 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 (κOA) increased from 0.058 at 30 nm to 0.09 at 200 nm, suggesting a higher oxidation state of OA at larger particle sizes, supported by a higher fraction of extremely low volatile OA (ELVOA) for larger size particles. Significantly different diurnal patterns of κOA were observed between Aitken mode and accumulation mode. For Aitken mode (30–100 nm), the κOA values showed daily minima (0.02–0.07) during daytime, while exhibited a daytime peak (~0.09) in the accumulation mode. 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 were 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 κOA value (0.1) could lead to an overestimation of the CCN number concentration (NCCN) up to 12 %–19 % at 0.1 %–0.7 % supersaturation (SS), which was more obvious at higher SS during daytime. Better prediction of NCCN could be achieved by using size-resolved diurnal κOA, which indicates that the size-dependence and diurnal variations of κOA can strongly affect the NCCN at different SS. 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.

Mingfu Cai et al.

Status: final response (author comments only)

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'Comment on acp-2022-23', Anonymous Referee #1, 02 Mar 2022
    • AC1: 'Reply on RC1', Mingfu Cai, 19 Apr 2022
  • RC2: 'Comment on acp-2022-23', Anonymous Referee #2, 14 Mar 2022
    • AC2: 'Reply on RC2', Mingfu Cai, 19 Apr 2022

Mingfu Cai et al.

Data sets

Distinct size dependence and diurnal variation of OA hygroscopicity, volatility, and CCN activity at a rural site in the Pearl River Delta (PRD) region, China Cai, Mingfu; Huang, Shan; Liu, Li

Mingfu Cai et al.


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Short summary
This study investigated the size dependence and diurnal variation of organic aerosol hygroscopicity, volatility, and cloud condensation nuclei (CCN) activity. We found that the physical properties of OA could vary in a large range at different particle sizes and affected the number concentration of CCN (NCCN) at all supersaturations. Our results highlight the importance of evaluating the atmospheric evolution processes of OA at different size ranges and their impact on climate effects.