Marine boundary layer aerosol in the eastern North Atlantic: seasonal variations and key controlling processes
Abstract
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 nm),accumulation (Ac, Dp within ~100 to ~300nm), andlarger accumulation (LA, nm) 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.
- Authors:
-
[1];
[2];
[3];
[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
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States); Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Biological and Environmental Research (BER); 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. https://doi.org/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. https://doi.org/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 = {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 Dp<~100nm),accumulation (Ac, Dp within ~100 to ~300nm), andlarger accumulation (LA, Dp>~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 = {Wed Dec 12 00:00:00 EST 2018},
month = {Wed Dec 12 00:00:00 EST 2018}
}
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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 »
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Works referencing / citing this record:
Nucleation-mode particle pool and large increases in N cn and N ccn observed over the northwestern Pacific Ocean in the spring of 2014
journal, January 2019
- Wang, Juntao; Shen, Yanjie; Li, Kai
- Atmospheric Chemistry and Physics, Vol. 19, Issue 13
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