Marine boundary layer aerosol in the eastern North Atlantic: seasonal variations and key controlling processes

Zheng, Guangjie; Wang, Yang; Aiken, Allison C.; Gallo, Francesca; Jensen, Michael P.; Kollias, Pavlos; Kuang, Chongai; Luke, Edward; Springston, Stephen; Uin, Janek; Wood, Robert; Wang, Jian

doi:10.5194/acp-18-17615-2018

Title: Marine boundary layer aerosol in the eastern North Atlantic: seasonal variations and key controlling processes

Journal Article · Wed Dec 12 00:00:00 EST 2018 · Atmospheric Chemistry and Physics (Online)

DOI:https://doi.org/10.5194/acp-18-17615-2018· OSTI ID:1485781

^[1]; Wang, Yang ^[1];

^[2]; Gallo, Francesca ^[2];

^[3]; Kollias, Pavlos ^[4]; Kuang, Chongai ^[3]; Luke, Edward ^[3];

^[3];

^[5];

^[1]

Brookhaven National Lab. (BNL), Upton, NY (United States). Environmental and Climate Science Dept.; Washington Univ., St. Louis, MO (United States). Center for Aerosol Science and Engineering, Dept. of Energy, Environmental and Chemical Engineering
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States). Environmental and Climate Science Dept.
Stony Brook Univ., NY (United States). School of Marine and Atmospheric Sciences
Univ. of Washington, Seattle, WA (United States). Dept. of Atmospheric Science

Abstract. The response of marine low cloud systems to changes in aerosol concentrationrepresents one of the largest uncertainties in climate simulations. Majorcontributions to this uncertainty are derived from poor understanding of aerosolunder natural conditions and the perturbation by anthropogenic emissions. Theeastern North Atlantic (ENA) is a region of persistent but diverse marineboundary layer (MBL) clouds, whose albedo and precipitation are highlysusceptible to perturbations in aerosol properties. In this study, we examineMBL aerosol properties, trace gas mixing ratios, and meteorologicalparameters measured at the Atmospheric Radiation Measurement Climate ResearchFacility's ENA site on Graciosa Island, Azores, Portugal, during a 3-yearperiod from 2015 to 2017. Measurements impacted by local pollution onGraciosa Island and during occasional intense biomass burning and dust eventsare excluded from this study. Submicron aerosol size distribution typicallyconsists of three modes: Aitken (At, diameter $D_{p} < ~ 100$ nm),accumulation (Ac, D_p within ~100 to ~300nm), andlarger accumulation (LA, $D_{p} > ~ 300$ nm) modes, with averagenumber concentrations (denoted as N_At, N_Ac, andN_LA below) of 330, 114, and 14cm^-3, respectively.N_At, N_Ac, and N_LA show contrasting seasonalvariations, suggesting different sources and removal processes.N_LA is dominated by sea spray aerosol (SSA) and is higher in winter andlower in summer. This is due to the seasonal variations of SSA production,in-cloud coalescence scavenging, and dilution by entrained free troposphere(FT) air. In comparison, SSA typically contributes a relatively minorfraction to N_At (10%) and N_Ac (21%) on an annual basis. Inaddition to SSA, sources of Ac-mode particles include entrainment of FTaerosols and condensation growth of Aitken-mode particles inside the MBL, whilein-cloud coalescence scavenging is the major sink of N_Ac. The observedseasonal variation of N_Ac, being higher in summer and lower in winter,generally agrees with the steady-state concentration estimated from majorsources and sinks. N_At is mainly controlled by entrainment of FTaerosol, coagulation loss, and growth of Aitken-mode particles into theAc-mode size range. Our calculation suggests that besides the directcontribution from entrained FT Ac-mode particles, growth of entrained FTAitken-mode particles in the MBL also represent a substantial source ofcloud condensation nuclei (CCN), with the highest contribution potentiallyreaching 60% during summer. The growth of Aitken-mode particles to CCN sizeis an expected result of the condensation of sulfuric acid, a product fromdimethyl sulfide oxidation, suggesting that ocean ecosystems may have asubstantial influence on MBL CCN populations in the ENA.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States); Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER); USDOE Office of Science (SC). Biological and Environmental Research (BER) (SC-23)

Grant/Contract Number:: SC0012704; SC0013489; AC02-98CH10886; 89233218CNA000001

OSTI ID:: 1485781

Alternate ID(s):: OSTI ID: 1507339

Report Number(s):: BNL-209680-2018-JAAM; LA-UR-19-20442

Journal Information:: Atmospheric Chemistry and Physics (Online), Vol. 18, Issue 23; ISSN 1680-7324

Publisher:: European Geosciences UnionCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 43 works

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Nucleation-mode particle pool and large increases in N cn and N ccn observed over the northwestern Pacific Ocean in the spring of 2014 Wang, Juntao; Shen, Yanjie; Li, Kai Atmospheric Chemistry and Physics, Vol. 19, Issue 13 https://doi.org/10.5194/acp-19-8845-2019	journal	January 2019

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Related Subjects

54 ENVIRONMENTAL SCIENCES
Earth Sciences
aerosol
cloud
condensation nuclei
seasonal variation
low marine cloud systems
Azores
Atmospheric Radiation Measurement
Eastern North Atlantic