On the differences in the vertical distribution of modeled aerosol optical depth over the southeastern Atlantic

Journal Article · Wed Apr 12 00:00:00 EDT 2023 · Atmospheric Chemistry and Physics (Online)

DOI:https://doi.org/10.5194/acp-23-4283-2023· OSTI ID:1969583

Chang, Ian; Gao, Lan; Flynn, Connor J.; Shinozuka, Yohei; Doherty, Sarah J.; Diamond, Michael S.; Longo, Karla M.; Ferrada, Gonzalo A.; Carmichael, Gregory R.; Castellanos, Patricia; da Silva, Arlindo M.; Saide, Pablo E.; Howes, Calvin; Xue, Zhixin; Mallet, Marc; Govindaraju, Ravi; Wang, Qiaoqiao; Cheng, Yafang; Feng, Yan; Burton, Sharon P. ; Ferrare, Richard A.; LeBlanc, Samuel E.; Kacenelenbogen, Meloë S.; Pistone, Kristina; Segal-Rozenhaimer, Michal; Meyer, Kerry G.; Ryoo, Ju-Mee; Pfister, Leonhard; Adebiyi, Adeyemi A.; Wood, Robert; Zuidema, Paquita; Christopher, Sundar A.; Redemann, Jens

Abstract. The southeastern Atlantic is home to an expansive smoke aerosol plume overlying a large cloud deck for approximately a third of the year. The aerosol plume is mainly attributed to the extensive biomass burning activities that occur in southern Africa. Current Earth system models (ESMs) reveal significant differences in their estimates of regional aerosol radiative effects over this region. Such large differences partially stem from uncertainties in the vertical distribution of aerosols in the troposphere. These uncertainties translate into different aerosol optical depths (AODs) in the planetary boundary layer (PBL) and the free troposphere (FT). This study examines differences of AOD fraction in the FT and AOD differences among ESMs (WRF-CAM5, WRF-FINN, GEOS-Chem, EAM-E3SM, ALADIN, GEOS-FP, and MERRA-2) and aircraft-based measurements from the NASA ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES) field campaign. Models frequently define the PBL as the well-mixed surface-based layer, but this definition misses the upper parts of decoupled PBLs, in which most low-level clouds occur. To account for the presence of decoupled boundary layers in the models, the height of maximum vertical gradient of specific humidity profiles from each model is used to define PBL heights. Results indicate that the monthly mean contribution of AOD in the FT to the total-column AOD ranges from 44 % to 74 % in September 2016 and from 54 % to 71 % in August 2017 within the region bounded by 25∘ S–0∘ N–S and 15∘ W–15∘ E (excluding land) among the ESMs. ALADIN and GEOS-Chem show similar aerosol plume patterns to a derived above-cloud aerosol product from the Moderate Resolution Imaging Spectroradiometer (MODIS) during September 2016, but none of the models show a similar above-cloud plume pattern to MODIS in August 2017. Using the second-generation High Spectral Resolution Lidar (HSRL-2) to derive an aircraft-based constraint on the AOD and the fractional AOD, we found that WRF-CAM5 produces 40 % less AOD than those from the HSRL-2 measurements, but it performs well at separating AOD fraction between the FT and the PBL. AOD fractions in the FT for GEOS-Chem and EAM-E3SM are, respectively, 10 % and 15 % lower than the AOD fractions from the HSRL-2. Their similar mean AODs reflect a cancellation of high and low AOD biases. Compared with aircraft-based observations, GEOS-FP, MERRA-2, and ALADIN produce 24 %–36 % less AOD and tend to misplace more aerosols in the PBL. The models generally underestimate AODs for measured AODs that are above 0.8, indicating their limitations at reproducing high AODs. The differences in the absolute AOD, FT AOD, and the vertical apportioning of AOD in different models highlight the need to continue improving the accuracy of modeled AOD distributions. These differences affect the sign and magnitude of the net aerosol radiative forcing, especially when aerosols are in contact with clouds.

• Research Organization: Argonne National Laboratory (ANL), Argonne, IL (United States)
• Sponsoring Organization: National Aeronautic and Space Administration (NASA); USDOE Office of Environmental Management (EM); USDOE Office of Science (SC), Biological and Environmental Research (BER); University of Oklahoma
• Grant/Contract Number: AC02-06CH11357
• OSTI ID: 1969583
• Alternate ID(s): OSTI ID: 2280944
• Journal Information: Atmospheric Chemistry and Physics (Online), Journal Name: Atmospheric Chemistry and Physics (Online) Journal Issue: 7 Vol. 23; ISSN 1680-7324
• Publisher: Copernicus GmbH
• Country of Publication: Germany
• Language: English

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54 ENVIRONMENTAL SCIENCES