Vertical profiles of trace gas and aerosol properties over the eastern North Atlantic: variations with season and synoptic condition

Wang, Yang; Zheng, Guangjie; Jensen, Michael P.; Knopf, Daniel A.; Laskin, Alexander; Matthews, Alyssa A.; Mechem, David; Mei, Fan; Moffet, Ryan; Sedlacek, Arthur J.; Shilling, John E.; Springston, Stephen; Sullivan, Amy; Tomlinson, Jason; Veghte, Daniel; Weber, Rodney; Wood, Robert; Zawadowicz, Maria A.; Wang, Jian

doi:10.5194/acp-21-11079-2021

Title: Vertical profiles of trace gas and aerosol properties over the eastern North Atlantic: variations with season and synoptic condition

Journal Article · Thu Jul 22 00:00:00 EDT 2021 · Atmospheric Chemistry and Physics (Online)

DOI:https://doi.org/10.5194/acp-21-11079-2021· OSTI ID:1809099

;

; Mechem, David;

;

; Sullivan, Amy;

; Veghte, Daniel;

;

Because of their extensive coverage, marine low clouds greatly impact the global climate. Presently, the response of marine low clouds to the changes in atmospheric aerosols remains a major source of uncertainty in climate simulations. One key contribution to this large uncertainty derives from the poor understanding of the properties and processes of marine aerosols under natural conditions and the perturbation by anthropogenic emissions. The eastern North Atlantic (ENA) is a region of persistent but diverse subtropical marine boundary layer (MBL) clouds, where cloud albedo and precipitation are highly susceptible to perturbations in aerosol properties. Here we examine the key processes that drive the cloud condensation nuclei (CCN) population in the MBL using comprehensive characterizations of aerosol and trace gas vertical profiles during the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) field campaign. During ACE-ENA, a total of 39 research flights were conducted in the Azores: 20 during summer 2017 and 19 during winter 2018. During summer, long-range-transported aerosol layers were periodically observed in the lower free troposphere (FT), leading to elevated FT CCN concentrations (N_CCN). Both biomass burning and pollution from North America contribute to submicron aerosol mass in these layers, with pollution likely the dominant contributor. In contrast, long-range transported continental emissions have a much weaker influence on the aerosol properties in the ENA during the winter season. While the entrainment of FT air is a major source of particle number in the MBL for both seasons, on average it does not serve as a direct source of CCN in the MBL because the average FT NCCN is the same or even lower than that in the MBL. The particle number flux due to FT entrainment is dominated by pre-CCN (particles that are too small to form cloud droplets under typical conditions, i.e., particles with sizes below the Hoppel minimum) due to the elevated Npre-CCN in the lower FT. Once these pre-CCN are entrained into the MBL, they can grow and reach CCN size range through condensational growth, representing an indirect and major source of MBL CCN in the ENA. The impact of synoptic conditions on the aerosol properties is examined. Under pre-front and post-front conditions, shallow convective activity often leads to a deep and decoupled boundary layer. Coalescence scavenging and evaporation of drizzle below clouds lead to reduced NCCN and larger accumulation-mode particle sizes in the upper cloud-containing decoupled layer, indicating that surface measurements overestimate the NCCN relevant to the formation of MBL clouds under decoupled conditions.

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Research Organization:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Atmospheric Radiation Measurement (ARM) Data Center; Brookhaven National Laboratory (BNL), Upton, NY (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Washington Univ., St. Louis, MO (United States)

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

Contributing Organization:: Pacific Northwest National Lab. (PNNL); Brookhaven National Lab. (BNL); Argonne National Lab. (ANL)

Grant/Contract Number:: SC0016370; AC05-76RL01830; SC0018948; SC0012704; SC0013489; KP1701000/57131; SC0020259; SC0021256; KP1701010

OSTI ID:: 1809099

Alternate ID(s):: OSTI ID: 1812369; OSTI ID: 1813332; OSTI ID: 1820147; OSTI ID: 1837835

Report Number(s):: BNL-221968-2021-JAAM; PNNL-SA-161330

Journal Information:: Atmospheric Chemistry and Physics (Online), Journal Name: Atmospheric Chemistry and Physics (Online) Vol. 21 Journal Issue: 14; ISSN 1680-7324

Publisher:: Copernicus GmbHCopyright Statement

Country of Publication:: Germany

Language:: English

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