Preprints
https://doi.org/10.5194/egusphere-2024-1347
https://doi.org/10.5194/egusphere-2024-1347
10 Jun 2024
 | 10 Jun 2024
Status: this preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).

Burning conditions and transportation pathways determine biomass-burning aerosol properties in the Ascension Island marine boundary layer

Amie Dobracki, Ernie Lewis, Arthur Sedlacek III, Tyler Tatro, Maria Zawadowicz, and Paquita Zuidema

Abstract. African biomass-burning aerosol (BBA) in the southeast Atlantic Ocean (SEA) marine boundary layer (MBL) is an important contributor to Earth’s radiation budget yet its representation remains poorly constrained in regional and global climate models. Data from the Layered Atlantic Smoke Interactions with Clouds (LASIC) field campaign on Ascension Island (‑7.95° N, ‑14.36° E) detail how fire source regions (burning conditions and fuel type), transport pathways, and longer-term chemical processing affect the chemical, microphysical, and optical properties of the BBA in the remote MBL between June and September of 2017. Ten individual plume events characterize the seasonal evolution of BBA characteristics. Inefficient burning conditions, determined by the mass ratio of refractory black carbon to above-background carbon monoxide (rBC:ΔCO), enhance organic- and sulfate-rich aerosol concentrations in June–July. In contrast, the heart of the burning season exhibited higher rBC:ΔCO values indicative of efficient burning conditions, correlating with more rBC-enriched BBA. Toward the end of the burning season, a mix of burning conditions results in increased variation of the BBA properties. The BBA transit to Ascension Island was predominantly through slow-moving pathways in the MBL and lower free troposphere (FT), facilitating prolonged chemical transformations through heterogeneous and aqueous phase processes. Heterogeneous oxidation can persist for up to 10 days, resulting in a considerable decrease in organic aerosol (OA) mass. OA to rBC mass ratios (OA:rBC) in the MBL between 2 and 5 contrast to higher values of 5 to 15 observed in the nearby FT. Conversely, early-season aqueous-phase processes primarily contributed to aerosol oxidation and some aerosol production, but not appreciable aerosol removal. These two chemical processes yield more light-absorbing BBA in the MBL than in the FT and explain the notably low scattering albedo at 530 nm (SSA530) values (< 0.80) at Ascension Island. This study establishes a robust correlation between SSA530 and OA:rBC across both MBL and FT, underscoring the dependency of optical properties on chemical composition. These findings highlight how the interplay between chemical composition and atmospheric processing can be improved in global and regional climate models. Questions remain on the mixing of aerosols with different pathway histories, and on what accounts for the doubling of the mass absorption coefficient in the boundary layer.

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Amie Dobracki, Ernie Lewis, Arthur Sedlacek III, Tyler Tatro, Maria Zawadowicz, and Paquita Zuidema

Status: open (until 22 Jul 2024)

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Amie Dobracki, Ernie Lewis, Arthur Sedlacek III, Tyler Tatro, Maria Zawadowicz, and Paquita Zuidema
Amie Dobracki, Ernie Lewis, Arthur Sedlacek III, Tyler Tatro, Maria Zawadowicz, and Paquita Zuidema

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Short summary
Biomass-burning aerosol is commonly present in the marine boundary layer of the southeast Atlantic Ocean between June and October. Our research indicates that burning conditions, aerosol transport pathways, and prolonged oxidation processes, both heterogeneous and aqueous-phase determine the chemical, microphysical, and optical properties of the boundary layer aerosol. Notably, we find that the aerosol optical properties can be estimated from the chemical properties alone.