Preprints
https://doi.org/10.5194/acp-2022-752
https://doi.org/10.5194/acp-2022-752
14 Nov 2022
 | 14 Nov 2022
Status: a revised version of this preprint was accepted for the journal ACP.

Impact of aerosol optics on vertical distribution of ozone

Shuqi Yan, Bin Zhu, Shuangshuang Shi, Wen Lu, Jinhui Gao, Hanqing Kang, and Duanyang Liu

Abstract. Tropospheric ozone, an important secondary pollutant, is greatly impacted by aerosols within boundary layer (BL). Previous studies have mainly attributed ozone variation to either aerosol-BL or aerosol-photolysis interactions at near surface. In this study, we analyze the sensitivities of ozone response to aerosol mixing states (e.g., mixing behaviour hypothesis of scattering and absorbing components) in the vertical direction and address the effects of aerosol-BL and aerosol-photolysis interactions on ozone profiles by WRF-Chem simulations. The aerosol internal mixing state experiment reasonably reproduces the vertical distribution and time variation of meteorological elements and ozone. Sensitive experiments show that aerosols lead to turbulent suppression, precursor accumulation, lower-level photolysis reduction and upper-level photolysis enhancement. Consequently, ozone basically decreases within entire BL during daytime (08:00~17:00), and the decrease is the least in external mixing state (0.6 %) compared with internal (9.8 %) and core-shell mixing states (7.4 %). The photolysis enhancement is the most significant in external mixing state due to its strong scattering ability. By process analysis, lower-level ozone chemical loss is enhanced due to photolysis reduction and NOX accumulation under VOC-limited regime. Upper-level ozone chemical production is accelerated due to higher photolysis rate resulting from aerosol backscattering. Therefore, the increased ozone entrainment from aloft BL to surface induced by boosted ozone vertical gradient outweighs the decreased ozone entrainment induced by turbulent suppression after 11:00 am. Additional simulations support that aerosol effect on precursor, photolysis and ozone is consistent under different underlying surface and pollution conditions.

Shuqi Yan 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-2022-752', Anonymous Referee #1, 30 Nov 2022
    • AC1: 'Reply on RC1', Shuqi Yan, 25 Feb 2023
  • RC2: 'Comment on acp-2022-752', Anonymous Referee #2, 03 Jan 2023
    • AC2: 'Reply on RC2', Shuqi Yan, 25 Feb 2023

Shuqi Yan et al.

Shuqi Yan et al.

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Short summary
We analyze the ozone response to aerosol mixing states in the vertical direction by WRF-Chem simulations. Aerosols generally lead to turbulent suppression, precursor accumulation, low-level photolysis reduction and upper-level photolysis enhancement under different underlying surface and pollution conditions. Consequently, ozone basically decreases within entire BL during daytime, and the decrease is the least in aerosol external mixing state compared with internal and core-shell mixing states.
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