04 Jun 2021

04 Jun 2021

Review status: this preprint is currently under review for the journal ACP.

Reduced volatility of aerosols from surface emission to the top of planetary boundary layer

Quan Liu1,3, Dantong Liu2, Yangzhou Wu2, Kai Bi1, Wenkang Gao4, Ping Tian1, Delong Zhao1, Siyuan Li2, Chenjie Yu5, Yunfei Wu6, Kang Hu2, Shuo Ding2, Qian Gao1, Fei Wang1, Hui He1,7, Mengyu Huang1,7, and Deping Ding1 Quan Liu et al.
  • 1Beijing Weather Modification Office, Beijing 100089, China
  • 2Department of Atmospheric Sciences, School of Earth Sciences, Zhejiang University, Hangzhou, Zhejiang, 310027, China
  • 3State Key Laboratory of Severe Weather & Key Laboratory of Atmospheric Chemistry of CMA, Chinese Academy of Meteorological Sciences, Beijing 100081, China
  • 4State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China
  • 5Centre for Atmospheric Sciences, School of Earth and Environmental Sciences, University of Manchester, Manchester M13 9PL, UK
  • 6Key Laboratory of Middle Atmosphere and Global Environment Observation (LAGEO), Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China
  • 7Field experiment base of cloud and precipitation research in North China, China Meteorological Administration, Beijing, 101200, China

Abstract. Aerosols from surface emission can be transported upwards through convective mixing in the planetary boundary layer (PBL), subsequently interacting with clouds, serving important sources to nucleate droplets or ice particles. However, the evolution of aerosol composition during this vertical transport has yet to be explicitly understood. In this study, simultaneous measurements of detailed aerosol compositions were conducted at both sites of urban Beijing (50 m a.s.l.) and HaiTuo mountain (1344 m a.s.l.) during wintertime, representing the anthropogenically polluted surface environment and the top of PBL respectively. The pollutants from surface emissions were observed to reach the mountain site on daily basis through daytime PBL connective mixing. From surface to the top of PBL, we found efficient transport or formation for lower-volatile species (black carbon, sulphate and low-volatile organic aerosol, OA); however notable reduction of semi-volatile substances, such as the fractions of nitrate and semi-volatile OA reduced by 74 % and 76 % respectively, during the upward transport. This implied the evaporation process may have occurred, in repartitioning the condensed semi-volatile substances to gas-phase, when aerosols were transported and exposed to a cleaner environment. Combining with the oxidation processes, these led to enhanced oxidation state of OA at the top of the PBL compared to surface environment, with an increase of oxygen to carbon atomic ratio by 0.2. Such reduction of aerosol volatility during vertical transport may be important in modifying its viscosity, nucleation activity and atmospheric lifetime.

Quan Liu et al.

Status: open (until 16 Jul 2021)

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Quan Liu et al.


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Short summary
Through simultaneous online measurements of detailed aerosol compositions at both surface and surface-influenced mountain sites, the evolution of aerosol composition during daytime vertical transport was investigated. The results show that from surface to the top of the PBL, the oxidation state of organic aerosol had been significantly enhanced due to evaporation and further oxidation on these evaporated gases.