Preprints
https://doi.org/10.5194/egusphere-2024-4135
https://doi.org/10.5194/egusphere-2024-4135
03 Feb 2025
 | 03 Feb 2025
Status: this preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).

The effect of organic nucleation on the indirect radiative forcing with a semi-explicit chemical mechanism for highly oxygenated organic molecules (HOMs)

Xinyue Shao, Minghuai Wang, Xinyi Dong, Yaman Liu, Stephen R. Arnold, Leighton A. Regayre, Duseong S. Jo, Wenxiang Shen, Hao Wang, Man Yue, Jingyi Wang, Wenxin Zhang, and Ken S. Carslaw

Abstract. Highly oxygenated organic molecules (HOMs) can significantly contribute to new particle formation (NPF). HOMs-derived NPF in preindustrial (PI) environments provides the baseline for calculating radiative forcing, yet global model studies examining this are lacking. Here, we use a global climate model with a semi-explicit HOMs chemistry and the associated nucleation scheme to systematically quantify the effect of HOMs-derived NPF on CCN formation and effective radiative forcing due to aerosol–cloud interactions (ERFaci). The improved model shows better agreement with measured cloud condensation nuclei (CCN) numbers. Aerosols generated from organic NPF nearly double the globally averaged CCN burden in PI (39 %) compared to PD (18 %) experiments. This weakens the ERFaci by 0.4 W m-2, corresponding to a 16 % reduction, with most of this reduction occurring in tropical regions where pure organic nucleation rates shows larger value in PI atmosphere. Unlike the findings of Gordon et al. (2016), the reduction is mainly driven by a greater enhancement of the sub-20 nm growth rate (GR) in the PI atmosphere compared to PD instead of the ~1 nm nucleation rate (j1.7nm). The greater enhancement of GR is due to higher HOM concentrations in the PI atmosphere, while the greater j1.7nm in PD environment results from higher sulfuric acid concentrations, leading to higher heteromolecular nucleation rates involving sulfuric acid and organics. The reduction underscores the critical role of biogenic NPF in CCN formation, particularly in the PI climate when cloud droplet concentrations and albedo are more sensitive to aerosol changes.

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Xinyue Shao, Minghuai Wang, Xinyi Dong, Yaman Liu, Stephen R. Arnold, Leighton A. Regayre, Duseong S. Jo, Wenxiang Shen, Hao Wang, Man Yue, Jingyi Wang, Wenxin Zhang, and Ken S. Carslaw

Status: open (until 17 Mar 2025)

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Xinyue Shao, Minghuai Wang, Xinyi Dong, Yaman Liu, Stephen R. Arnold, Leighton A. Regayre, Duseong S. Jo, Wenxiang Shen, Hao Wang, Man Yue, Jingyi Wang, Wenxin Zhang, and Ken S. Carslaw
Xinyue Shao, Minghuai Wang, Xinyi Dong, Yaman Liu, Stephen R. Arnold, Leighton A. Regayre, Duseong S. Jo, Wenxiang Shen, Hao Wang, Man Yue, Jingyi Wang, Wenxin Zhang, and Ken S. Carslaw

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Short summary
This study uses a global chemistry-climate model to investigate how new particle formation (NPF) from highly oxygenated organic molecules (HOMs) contributes to cloud condensation nuclei (CCN) in both preindustrial (PI) and present-day (PD) environments, and its impact on aerosol indirect radiative forcing. The findings highlight the crucial role of biogenic emissions in climate change, providing new insights for carbon-neutral scenarios and enhancing understanding of aerosol-cloud interactions.
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