On the differences in the vertical distribution of modeled aerosol optical depth over the southeast Atlantic
Authors: 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 
Published: September 2022

Abstract. The southeast 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 activity that occurs 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 (AOD) 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° and 15°W–15°E (excluding land) among the ESMs. 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 and their similarities in the mean AODs are the result of cancellation of high and low AOD biases. GEOS-FP, MERRA-2, and ALADIN produce 24 %–36 % less AOD and tend to misplace more aerosols in the PBL compared to aircraft-based observations. 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.