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

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 <~100 nm),accumulation (Ac, D p within ~100 to ~300nm), andlarger accumulation (LA, D p &gt; ~ 300 nm) modes, with averagenumber concentrations (denoted as N At, N Ac, and N 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.

Authors:
ORCiD logo [1];  [1]; ORCiD logo [2];  [2]; ORCiD logo [3];  [4];  [3];  [3]; ORCiD logo [3]; ORCiD logo [3]; ORCiD logo [5]; ORCiD logo [1]
  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
  2. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  3. Brookhaven National Lab. (BNL), Upton, NY (United States). Environmental and Climate Science Dept.
  4. Stony Brook Univ., NY (United States). School of Marine and Atmospheric Sciences
  5. Univ. of Washington, Seattle, WA (United States). Dept. of Atmospheric Science
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States); USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23); USDOE Office of Science (SC). Biological and Environmental Research (BER) (SC-23)
OSTI Identifier:
1485781
Alternate Identifier(s):
OSTI ID: 1507339
Report Number(s):
BNL-209680-2018-JAAM; LA-UR-19-20442
Journal ID: ISSN 1680-7324
Grant/Contract Number:  
SC0012704; SC0013489; AC02-98CH10886; 89233218CNA000001
Resource Type:
Accepted Manuscript
Journal Name:
Atmospheric Chemistry and Physics (Online)
Additional Journal Information:
Journal Name: Atmospheric Chemistry and Physics (Online); Journal Volume: 18; Journal Issue: 23; Journal ID: ISSN 1680-7324
Publisher:
European Geosciences Union
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; Earth Sciences; aerosol, cloud, condensation nuclei, seasonal variation, low marine cloud systems, Azores, Atmospheric Radiation Measurement, Eastern North Atlantic

Citation Formats

Zheng, Guangjie, Wang, Yang, Aiken, Allison C., Gallo, Francesca, Jensen, Michael P., Kollias, Pavlos, Kuang, Chongai, Luke, Edward, Springston, Stephen, Uin, Janek, Wood, Robert, and Wang, Jian. Marine boundary layer aerosol in the eastern North Atlantic: seasonal variations and key controlling processes. United States: N. p., 2018. Web. doi:10.5194/acp-18-17615-2018.
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. Marine boundary layer aerosol in the eastern North Atlantic: seasonal variations and key controlling processes. United States. doi:10.5194/acp-18-17615-2018.
Zheng, Guangjie, Wang, Yang, Aiken, Allison C., Gallo, Francesca, Jensen, Michael P., Kollias, Pavlos, Kuang, Chongai, Luke, Edward, Springston, Stephen, Uin, Janek, Wood, Robert, and Wang, Jian. Wed . "Marine boundary layer aerosol in the eastern North Atlantic: seasonal variations and key controlling processes". United States. doi:10.5194/acp-18-17615-2018. https://www.osti.gov/servlets/purl/1485781.
@article{osti_1485781,
title = {Marine boundary layer aerosol in the eastern North Atlantic: seasonal variations and key controlling processes},
author = {Zheng, Guangjie and Wang, Yang and Aiken, Allison C. and Gallo, Francesca and Jensen, Michael P. and Kollias, Pavlos and Kuang, Chongai and Luke, Edward and Springston, Stephen and Uin, Janek and Wood, Robert and Wang, Jian},
abstractNote = {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 <~100 nm),accumulation (Ac, Dp within ~100 to ~300nm), andlarger accumulation (LA, Dp&gt;~300nm) modes, with averagenumber concentrations (denoted as NAt, NAc, andNLA below) of 330, 114, and 14cm-3, respectively.NAt, NAc, and NLA show contrasting seasonalvariations, suggesting different sources and removal processes.NLA 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 NAt (10%) and NAc (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 NAc. The observedseasonal variation of NAc, being higher in summer and lower in winter,generally agrees with the steady-state concentration estimated from majorsources and sinks. NAt 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.},
doi = {10.5194/acp-18-17615-2018},
journal = {Atmospheric Chemistry and Physics (Online)},
number = 23,
volume = 18,
place = {United States},
year = {2018},
month = {12}
}

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Figures / Tables:

Figure 1 Figure 1: Cluster analysis of 10-day back-trajectories arriving at 100 m above the ENA site in different seasons. The analysis was conducted using the Hybrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT) 4 model (Stein et al., 2015). The 10-day back trajectories were simulated with a time step of 6 hours usingmore » National Centers for Environmental Prediction (NCEP) Global Data Assimilation System (GDAS) meteorological data as input. A cluster analysis of these trajectories was then performed, and for each season, the solution that captures most of the variance (e.g., Abdalmogith and Harrison (2005)) and with less than 5 identified clusters is chosen. The average trajectories of the clusters are represented by different colors, and the associated numbers denoted the arbitrarily given cluster ID and the occurrence percentages of this cluster. For example, number of 1 (90 %) beside the red trajectories indicated that the No. 1 cluster has an average trajectory shown by the red lines, and at 90 % times the air masses arriving at the ENA site belong to this cluster.« less

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Microlayer source of oxygenated volatile organic compounds in the summertime marine Arctic boundary layer
journal, May 2017

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Design and performance of a three-wavelength LED-based total scatter and backscatter integrating nephelometer
journal, January 2011

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Marine boundary layer measurements of new particle formation and the effects nonprecipitating clouds have on aerosol size distribution
journal, January 1994

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The importance of interstitial particle scavenging by cloud droplets in shaping the remote aerosol size distribution and global aerosol-climate effects
journal, January 2015

  • Pierce, J. R.; Croft, B.; Kodros, J. K.
  • Atmospheric Chemistry and Physics, Vol. 15, Issue 11
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Estimation of seasonal dimethyl sulphide fluxes over the North Atlantic Ocean and their contribution to European pollution levels
journal, January 1995

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Pollution and the planetary albedo
journal, December 1974


Trace gas concentrations and meteorology in rural Virginia: 1. Ozone and carbon monoxide
journal, January 1991

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Mixing height determination by ceilometer
journal, January 2006

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  • Atmospheric Chemistry and Physics, Vol. 6, Issue 6
  • DOI: 10.5194/acp-6-1485-2006

Precipitation driving of droplet concentration variability in marine low clouds: PRECIPITATION DRIVING OF DROP CONC
journal, October 2012

  • Wood, Robert; Leon, David; Lebsock, Matthew
  • Journal of Geophysical Research: Atmospheres, Vol. 117, Issue D19
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