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https://doi.org/10.5194/egusphere-2024-401
https://doi.org/10.5194/egusphere-2024-401
13 Feb 2024
 | 13 Feb 2024

Global modeling of aerosol nucleation with an explicit chemical mechanism for highly oxygenated organic molecules (HOMs)

Xinyue Shao, Minghuai Wang, Xinyi Dong, Yaman Liu, Wenxiang Shen, Stephen Arnold, Leighton Regayre, Meinrat Andreae, Mira Pöhlker, Duseong Jo, Man Yue, and Ken Carslaw

Abstract. New particle formation (NPF) involving organic compounds has been identified as an important process affecting aerosol particle number concentrations in the global atmosphere. Laboratory studies have shown that highly oxygenated organic molecules (HOMs) can make a substantial contribution to NPF, but there is a lack of global model studies of NPF with detailed HOMs chemistry. Here, we add a state-of-art biogenic HOMs chemistry scheme with 96 chemical reactions to a global chemistry-climate model and quantify the contribution to global aerosols through HOMs-driven NPF. The updated model captures the frequency of NPF events observed at continental surface sites (normalized mean bias changes from -96 % to -15 %) and shows reasonable agreement with measured rates of NPF and sub-20 nm particle growth. Sensitivity simulations show that the effect of HOMs on particle growth is more important for particle number than the effect on particle formation. Globally, organics contribute around 45 % of the annual mean vertically-integrated nucleation rate (at 1 nm) and 25 % of the vertically-averaged growth rate. The inclusion of HOMs-related processes leads to a 39 % increase in the global annual mean aerosol number burden and a 33 % increase in cloud condensation nuclei (CCN) burden at 0.5 % supersaturation compared to a simulation with only inorganic nucleation. Our work predicts a greater contribution of organic nucleation to NPF than previous studies due to the explicit HOMs mechanism and an updated inorganic NPF scheme. The large contribution of biogenic HOMs to NPF on a global scale could make global aerosol sensitive to changes in biogenic emissions.

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Xinyue Shao, Minghuai Wang, Xinyi Dong, Yaman Liu, Wenxiang Shen, Stephen Arnold, Leighton Regayre, Meinrat Andreae, Mira Pöhlker, Duseong Jo, Man Yue, and Ken Carslaw

Status: final response (author comments only)

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'Comment on egusphere-2024-401', Anonymous Referee #1, 12 Mar 2024
  • RC2: 'Comment on egusphere-2024-401', Anonymous Referee #2, 31 Mar 2024
Xinyue Shao, Minghuai Wang, Xinyi Dong, Yaman Liu, Wenxiang Shen, Stephen Arnold, Leighton Regayre, Meinrat Andreae, Mira Pöhlker, Duseong Jo, Man Yue, and Ken Carslaw
Xinyue Shao, Minghuai Wang, Xinyi Dong, Yaman Liu, Wenxiang Shen, Stephen Arnold, Leighton Regayre, Meinrat Andreae, Mira Pöhlker, Duseong Jo, Man Yue, and Ken Carslaw

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Short summary
Highly oxygenated organic molecules (HOMs) play an important role in atmospheric new particle formation (NPF). By explicitly coupling the chemical mechanism of HOMs and a comprehensive nucleation scheme in a global climate model. The updated model shows better agreement with measurements of nucleation rate, growth rate, NPF event frequency. Our results reveal that HOMs-driven NPF leads to a considerable increase in particle and cloud condensation nuclei burden globally.