Quantifying the impacts of marine aerosols over the southeast Atlantic Ocean using a chemical transport model: implications for aerosol–cloud interactions

Hossain, Mashiat; Garland, Rebecca M.; Horowitz, Hannah M.

doi:10.5194/acp-24-14123-2024

Title: Quantifying the impacts of marine aerosols over the southeast Atlantic Ocean using a chemical transport model: implications for aerosol–cloud interactions

Journal Article · 18 December 2024 · Atmospheric Chemistry and Physics (Online)

DOI: https://doi.org/10.5194/acp-24-14123-2024 · OSTI ID:2484033

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Univ. of Illinois at Urbana-Champaign, IL (United States)
Univ. of Pretoria (South Africa)

The southeast Atlantic region, characterized by persistent stratocumulus clouds, has one of the highest uncertainties in aerosol radiative forcing and significant variability across climate models. In this study, we analyze the seasonally varying role of marine aerosol sources and identify key uncertainties in aerosol composition at cloud-relevant altitudes over the southeast Atlantic using the GEOS-Chem chemical transport model. We evaluate simulated aerosol optical depth (AOD) and speciated aerosol concentrations against those collected from ground observations and aircraft campaigns such as LASIC, ORACLES, and CLARIFY, conducted during 2017. The model consistently underestimates AOD relative to AERONET, particularly at remote locations like Ascension Island. However, when compared with aerosol mass concentrations from aircraft campaigns during the biomass burning period, it performs adequately at cloud-relevant altitudes, with a normalized mean bias (NMB) between -3.5 % (CLARIFY) and -7.5 % (ORACLES). At these altitudes, in the model, organic aerosols (63 %) dominate during the biomass burning period, while sulfate (41 %) prevails during austral summer, when dimethylsulfide (DMS) emissions peak in the model. Our findings indicate that marine sulfate can account for up to 69 % of total sulfate during the high-DMS period. Sensitivity analyses indicate that refining DMS emissions and oxidation chemistry may increase sulfate aerosol produced from marine sources, highlighting that there remains large uncertainty as to the role of DMS emissions in the marine boundary layer. Additionally, we find marine primary organic aerosol emissions may substantially increase total organic aerosol concentrations, particularly during austral summer. This study underscores the imperative need to refine marine emissions and their chemical transformations, as aerosols from marine sources are a major component of total aerosols at cloud-relevant altitudes and may impact uncertainties in aerosol radiative forcing over the southeast Atlantic.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Atmospheric Radiation Measurement (ARM) Data Center

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER)

Contributing Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 2484033

Journal Information:: Atmospheric Chemistry and Physics (Online), Journal Name: Atmospheric Chemistry and Physics (Online) Journal Issue: 24 Vol. 24; ISSN 1680-7324

Publisher:: Copernicus Publications, EGUCopyright Statement

Country of Publication:: United States

Language:: English

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