Modeling the smoky troposphere of the southeast Atlantic: A comparison to ORACLES airborne observations from September of 2016

Yohei Shinozuka, Pablo E. Saide, Gonzalo A. Ferrada, Sharon P. Burton, Richard Ferrare, Sarah J. Doherty, Hamish Gordon, Karla Longo, Marc Mallet, Yan Feng, Qiaoqiao Wang, Yafang Cheng, Amie Dobracki, Steffen Freitag, Steven G. Howell, Samuel Leblanc, Connor Flynn, Michal Segal-Rosenhaimer, Kristina Pistone, James R. PodolskeEric J. Stith, Joseph Ryan Bennett, Gregory R. Carmichael, Arlindo Da Silva, Ravi Govindaraju, Ruby Leung, Yang Zhang, Leonhard Pfister, Ju Mee Ryoo, Jens Redemann, Robert Wood, Paquita Zuidema

Research output: Contribution to journalArticlepeer-review

13 Scopus citations

Abstract

In the southeast Atlantic, well-defined smoke plumes from Africa advect over marine boundary layer cloud decks; both are most extensive around September, when most of the smoke resides in the free troposphere. A framework is put forth for evaluating the performance of a range of global and regional atmospheric composition models against observations made during the NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) airborne mission in September 2016. A strength of the comparison is a focus on the spatial distribution of a wider range of aerosol composition and optical properties than has been done previously. The sparse airborne observations are aggregated into approximately 2 grid boxes and into three vertical layers: 3 6 km, the layer from cloud top to 3 km, and the cloudtopped marine boundary layer. Simulated aerosol extensive properties suggest that the flight-day observations are reasonably representative of the regional monthly average, with systematic deviations of 30% or less. Evaluation against observations indicates that all models have strengths and weaknesses, and there is no single model that is superior to all the others in all metrics evaluated. Whereas all six models typically place the top of the smoke layer within 0 500m of the airborne lidar observations, the models tend to place the smoke layer bottom 300 1400m lower than the observations. A spatial pattern emerges, in which most models underestimate the mean of most smoke quantities (black carbon, extinction, carbon monoxide) on the diagonal corridor between 16 S, 6 E, and 10 S, 0 E, in the 3 6 km layer, and overestimate them further south, closer to the coast, where less aerosol is present. Model representations of the abovecloud aerosol optical depth differ more widely. Most models overestimate the organic aerosol mass concentrations relative to those of black carbon, and with less skill, indicating model uncertainties in secondary organic aerosol processes. Regional-mean free-Tropospheric model ambient single scattering albedos vary widely, between 0.83 and 0.93 compared with in situ dry measurements centered at 0.86, despite minimal impact of humidification on particulate scattering. The modeled ratios of the particulate extinction to the sum of the black carbon and organic aerosol mass concentrations (a mass extinction efficiency proxy) are typically too low and vary too little spatially, with significant inter-model differences. Most models overestimate the carbonaceous mass within the offshore boundary layer. Overall, the diversity in the model biases suggests that different model processes are responsible. The wide range of model optical properties requires further scrutiny because of their importance for radiative effect estimates.

Original languageEnglish (US)
Article number2020
Pages (from-to)11491-11526
Number of pages36
JournalAtmospheric Chemistry and Physics
Volume20
Issue number19
DOIs
StatePublished - Oct 7 2020

ASJC Scopus subject areas

  • Atmospheric Science

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