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Title: Factors controlling marine aerosol size distributions and their climate effects over the northwest Atlantic Ocean region

Journal Article · · Atmospheric Chemistry and Physics (Online)

Abstract. Aerosols over Earth's remote and spatially extensive ocean surfaces have important influences on planetary climate. However, these aerosols and their effects remain poorly understood, in part due to the remoteness and limited observations over these regions. In this study, we seek to understand factors that shape marine aerosol size distributions and composition in the northwest Atlantic Ocean region. We use the GEOS-Chem model with the TwO-Moment Aerosol Sectional (TOMAS) microphysics algorithm model to interpret measurements collected from ship and aircraft during the four seasonal campaigns of the North Atlantic Aerosols and Marine Ecosystems Study (NAAMES) conducted between 2015 and 2018. Observations from the NAAMES campaigns show enhancements in the campaign-median number of aerosols with diameters larger than 3 nm in the lower troposphere (below 6 km), most pronounced during the phytoplankton bloom maxima (May/June) below 2 km in the free troposphere. Our simulations, combined with NAAMES ship and aircraft measurements, suggest several key factors that contribute to aerosol number and size in the northwest Atlantic lower troposphere, with significant regional-mean (40–60∘ N and 20–50∘ W) cloud-albedo aerosol indirect effect (AIE) and direct radiative effect (DRE) processes during the phytoplankton bloom. These key factors and their associated simulated radiative effects in the region include the following: (1) particle formation near and above the marine boundary layer (MBL) top (AIE: −3.37 W m−2, DRE: −0.62 W m−2); (2) particle growth due to marine secondary organic aerosol (MSOA) as the nascent particles subside into the MBL, enabling them to become cloud-condensation-nuclei-sized particles (AIE: −2.27 W m−2, DRE: −0.10 W m−2); (3) particle formation and growth due to the products of dimethyl sulfide, above and within the MBL (−1.29 W m−2, DRE: −0.06 W m−2); (4) ship emissions (AIE: −0.62 W m−2, DRE: −0.05 W m−2); and (5) primary sea spray emissions (AIE: +0.04 W m−2, DRE: −0.79 W m−2). Our results suggest that a synergy of particle formation in the lower troposphere (particularly near and above the MBL top) and growth by MSOA contributes strongly to cloud-condensation-nuclei-sized particles with significant regional radiative effects in the northwest Atlantic. To gain confidence in radiative effect magnitudes, future work is needed to understand (1) the sources and temperature dependence of condensable marine vapors forming MSOA, (2) primary sea spray emissions, and (3) the species that can form new particles in the lower troposphere and grow these particles as they descend into the marine boundary layer.

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Biological and Environmental Research (BER)
Contributing Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)
Grant/Contract Number:
SC0019000
OSTI ID:
1765063
Alternate ID(s):
OSTI ID: 1769283
Journal Information:
Atmospheric Chemistry and Physics (Online), Journal Name: Atmospheric Chemistry and Physics (Online) Vol. 21 Journal Issue: 3; ISSN 1680-7324
Publisher:
Copernicus Publications, EGUCopyright Statement
Country of Publication:
Germany
Language:
English

References (172)

A numerical scheme to calculate temperature and salinity dependent air-water transfer velocities for any gas journal January 2010
Enhanced New Particle Formation Above the Marine Boundary Layer Over the Yellow Sea: Potential Impacts on Cloud Condensation Nuclei journal April 2020
Primary and Secondary Organic Marine Aerosol and Oceanic Biological Activity: Recent Results and New Perspectives for Future Studies journal January 2010
Biogenically driven organic contribution to marine aerosol journal October 2004
Carbohydrate-like composition of submicron atmospheric particles and their production from ocean bubble bursting journal December 2009
Source and evolution of the marine aerosol-A new perspective: MARINE AEROSOL-A NEW PERSPECTIVE journal October 2005
Gas-particle partitioning of atmospheric Hg(II) and its effect on global mercury deposition journal January 2012
Important Source of Marine Secondary Organic Aerosol from Biogenic Amines journal December 2008
Growth of nucleation mode particles in the summertime Arctic: a case study journal January 2016
Reactions of Methanesulfonic Acid with Amines and Ammonia as a Source of New Particles in Air journal October 2015
Secondary organic aerosols over oceans via oxidation of isoprene and monoterpenes from Arctic to Antarctic journal July 2013
The case against climate regulation via oceanic phytoplankton sulphur emissions journal November 2011
Variations and sources of the equivalent black carbon in the high Arctic revealed by long-term observations at Alert and Barrow: 1989–2003 journal January 2006
Contribution of Arctic seabird-colony ammonia to atmospheric particles and cloud-albedo radiative effect journal November 2016
Production flux of sea spray aerosol journal January 2011
Effects of near-source coagulation of biomass burning aerosols on global predictions of aerosol size distributions and implications for aerosol radiative effects journal January 2019
Cluster activation theory as an explanation of the linear dependence between formation rate of 3nm particles and sulphuric acid concentration journal January 2006
Remote Sensing Retrieval of Isoprene Concentrations in the Southern Ocean journal July 2020
Interactions of fire emissions and urban pollution over California: Ozone formation and air quality simulations journal September 2012
Constraints from 210 Pb and 7 Be on wet deposition and transport in a global three-dimensional chemical tracer model driven by assimilated meteorological fields journal June 2001
Long-range transported North American wildfire aerosols observed in marine boundary layer of eastern North Atlantic journal June 2020
Modeling chemical and aerosol processes in the transition from closed to open cells during VOCALS-REx journal January 2011
Ocean-atmosphere trace gas exchange journal January 2012
Oxidation Products of Biogenic Emissions Contribute to Nucleation of Atmospheric Particles journal May 2014
Overview paper: New insights into aerosol and climate in the Arctic journal January 2019
Results from the DC-8 Inlet Characterization Experiment (DICE): Airborne Versus Surface Sampling of Mineral Dust and Sea Salt Aerosols journal February 2007
Ice-nucleating particles in Canadian Arctic sea-surface microlayer and bulk seawater journal January 2017
Parameterization for Atmospheric New-Particle Formation: Application to a System Involving Sulfuric Acid and Condensable Water-Soluble Organic Vapors journal October 2004
The scavenging processes controlling the seasonal cycle in Arctic sulphate and black carbon aerosol journal January 2012
Processes controlling the annual cycle of Arctic aerosol number and size distributions journal January 2016
DMS oxidation and sulfur aerosol formation in the marine troposphere: a focus on reactive halogen and multiphase chemistry journal January 2018
Global indirect aerosol effects: a review journal January 2005
Amplification of global warming through pH dependence of DMS production simulated with a fully coupled Earth system model journal January 2017
Observationally constrained analysis of sea salt aerosol in the marine atmosphere journal January 2019
Primary and secondary marine organic aerosols over the North Atlantic Ocean during the MAP experiment: ORGANIC AEROSOLS OVER NORTH ATLANTIC journal November 2011
Source attribution and interannual variability of Arctic pollution in spring constrained by aircraft (ARCTAS, ARCPAC) and satellite (AIRS) observations of carbon monoxide journal January 2010
Unravelling New Processes at Interfaces: Photochemical Isoprene Production at the Sea Surface journal October 2015
Sea Spray Aerosol: Where Marine Biology Meets Atmospheric Chemistry journal December 2018
Small fraction of marine cloud condensation nuclei made up of sea spray aerosol journal August 2017
Dimethyl sulfide control of the clean summertime Arctic aerosol and cloud journal December 2013
Free troposphere as a major source of CCN for the equatorial pacific boundary layer: long-range transport and teleconnections journal January 2013
An improved parameterization for sulfuric acid–water nucleation rates for tropospheric and stratospheric conditions journal January 2002
Model representations of aerosol layers transported from North America over the Atlantic Ocean during the Two-Column Aerosol Project: MODEL REPRESENTATIONS OF AEROSOL LAYERS journal August 2016
Marine boundary layer aerosol in the eastern North Atlantic: seasonal variations and key controlling processes journal January 2018
Variability in Marine Plankton Ecosystems Are Not Observed in Freshly Emitted Sea Spray Aerosol Over the North Atlantic Ocean journal January 2020
Advances in characterization of size-resolved organic matter in marine aerosol over the North Atlantic journal January 2004
Important global and regional differences in aerosol cloud-albedo effect estimates between simulations with and without prognostic aerosol microphysics: DIFFERENCES IN CLOUD-ALBEDO AEROSOL INDIRECT EFFECT journal April 2017
Measurements of air-sea gas transfer during an open ocean algal bloom journal July 2000
The potential role of methanesulfonic acid (MSA) in aerosol formation and growth and the associated radiative forcings journal January 2019
Global airborne sampling reveals a previously unobserved dimethyl sulfide oxidation mechanism in the marine atmosphere journal February 2020
Chemistry and Related Properties of Freshly Emitted Sea Spray Aerosol journal February 2015
A global anthropogenic emission inventory of atmospheric pollutants from sector- and fuel-specific sources (1970–2017): an application of the Community Emissions Data System (CEDS) journal January 2020
A backward modeling study of intercontinental pollution transport using aircraft measurements journal January 2003
Sea Spray Aerosol Formation: Laboratory Results on the Role of Air Entrainment, Water Temperature, and Phytoplankton Biomass journal October 2019
Sensitivity of cloud condensation nuclei to regional changes in dimethyl-sulphide emissions journal January 2013
Characterization of aerosol growth events over Ellesmere Island during the summers of 2015 and 2016 journal January 2019
Global fire emissions estimates during 1997–2016 journal January 2017
Field-Deployable, High-Resolution, Time-of-Flight Aerosol Mass Spectrometer journal December 2006
Dimethyl sulfide air-sea fluxes and biogenic sulfur as a source of new aerosols in the Arctic fall journal January 2011
The North Atlantic Aerosol and Marine Ecosystem Study (NAAMES): Science Motive and Mission Overview journal March 2019
Arctic marine secondary organic aerosol contributes significantly to summertime particle size distributions in the Canadian Arctic Archipelago journal January 2019
Single-particle measurements of midlatitude black carbon and light-scattering aerosols from the boundary layer to the lower stratosphere journal January 2006
Stratocumulus Clouds journal August 2012
A study of new particle formation in the marine boundary layer over the central Arctic Ocean using a flexible multicomponent aerosol dynamic model journal January 2012
Relating atmospheric and oceanic DMS levels to particle nucleation events in the Canadian Arctic journal January 2011
The aerosol radiative effects of uncontrolled combustion of domestic waste journal January 2016
Beyond SO x reductions from shipping: assessing the impact of NO x and carbonaceous-particle controls on human health and climate journal December 2020
Global distribution of sea salt aerosols: new constraints from in situ and remote sensing observations journal January 2011
Estimates of the direct and indirect radiative forcing due to tropospheric aerosols: A review journal November 2000
Distribution and Drivers of Marine Isoprene Concentration across the Southern Ocean journal May 2020
In situ evaluation of air-sea gas exchange parameterizations using novel conservative and volatile tracers journal March 2000
Observational evidence for the formation of DMS-derived aerosols during Arctic phytoplankton blooms journal January 2017
Cloud, precipitation and radiation responses to large perturbations in global dimethyl sulfide journal January 2018
Parameterization of surface resistances to gaseous dry deposition in regional-scale numerical models journal January 1989
Bringing the ocean into the laboratory to probe the chemical complexity of sea spray aerosol journal April 2013
Substantial Seasonal Contribution of Observed Biogenic Sulfate Particles to Cloud Condensation Nuclei journal February 2018
Factors driving the seasonal and hourly variability of sea-spray aerosol number in the North Atlantic journal September 2019
A compact PTR-ToF-MS instrument for airborne measurements of volatile organic compounds at high spatiotemporal resolution journal January 2014
Arctic shipping emissions inventories and future scenarios journal January 2010
A parameterization of aerosol activation 3. Sectional representation journal January 2002
Marine aerosol formation from biogenic iodine emissions journal June 2002
Observation of sea-salt fraction in sub-100 nm diameter particles at Cape Grim: Observation of sub-100 nm Cape Grim SSA journal March 2015
Regional marine boundary layer aerosol size distributions in the Indian, Atlantic, and Pacific Oceans: A comparison of INDOEX measurements with ACE-1, ACE-2, and Aerosols99 journal January 2002
Satellite-based estimate of global aerosol–cloud radiative forcing by marine warm clouds journal August 2014
The climate impact of ship NO x emissions: an improved estimate accounting for plume chemistry journal January 2014
A Fast and Efficient Version of the TwO-Moment Aerosol Sectional (TOMAS) Global Aerosol Microphysics Model journal June 2012
Impacts on cloud radiative effects induced by coexisting aerosols converted from international shipping and maritime DMS emissions journal January 2018
Large contribution of natural aerosols to uncertainty in indirect forcing journal November 2013
Processes Controlling the Composition and Abundance of Arctic Aerosol journal November 2018
Historical (1750–2014) anthropogenic emissions of reactive gases and aerosols from the Community Emissions Data System (CEDS) journal January 2018
An advanced modeling study on the impacts and atmospheric implications of multiphase dimethyl sulfide chemistry journal September 2016
The Model of Emissions of Gases and Aerosols from Nature version 2.1 (MEGAN2.1): an extended and updated framework for modeling biogenic emissions journal January 2012
An evaluation of global organic aerosol schemes using airborne observations journal January 2020
Summertime observations of elevated levels of ultrafine particles in the high Arctic marine boundary layer journal January 2017
Marine aerosol production: a review of the current knowledge
  • O'Dowd, Colin D.; de Leeuw, Gerrit
  • Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 365, Issue 1856 https://doi.org/10.1098/rsta.2007.2043
journal May 2007
Dimethyl Sulfide and Dimethyl Sulfoxide and Their Oxidation in the Atmosphere February 2006
A parameterization of sea-salt aerosol source function for sub- and super-micron particles: SEA-SALT AEROSOL PRODUCTION journal October 2003
Observed inter-relations between 10m winds, ocean whitecaps and marine aerosols journal April 1983
The sensitivity of Southern Ocean aerosols and cloud microphysics to sea spray and sulfate aerosol production in the HadGEM3-GA7.1 chemistry–climate model journal January 2019
Long-term trends of the black carbon concentrations in the Canadian Arctic journal January 2004
A review of natural aerosol interactions and feedbacks within the Earth system journal January 2010
Parametrization of ternary nucleation rates for H 2 SO 4 -NH 3 -H 2 O vapors journal January 2002
Source attribution of Arctic black carbon constrained by aircraft and surface measurements journal January 2017
Mineral Dust Entrainment and Deposition (DEAD) model: Description and 1990s dust climatology journal January 2003
Intercontinental air pollution transport from North America to Europe: Experimental evidence from airborne measurements and surface observations journal January 2005
Mortality from Ship Emissions: A Global Assessment journal December 2007
A marine biogenic source of atmospheric ice-nucleating particles journal September 2015
PM and light extinction model performance metrics, goals, and criteria for three-dimensional air quality models journal August 2006
Air-Sea exchange of biogenic volatile organic compounds and the impact on aerosol particle size distributions: Air-Sea Exchange of Biogenic VOCs journal April 2017
Arctic aerosol life cycle: linking aerosol size distributions observed between 2000 and 2010 with air mass transport and precipitation at Zeppelin station, Ny-Ålesund, Svalbard journal January 2013
Atmospheric DMS in the Arctic Ocean and Its Relation to Phytoplankton Biomass journal March 2018
Natural aerosols explain seasonal and spatial patterns of Southern Ocean cloud albedo journal July 2015
Accounting for non-linear chemistry of ship plumes in the GEOS-Chem global chemistry transport model journal January 2011
Sources of carbonaceous aerosols and deposited black carbon in the Arctic in winter-spring: implications for radiative forcing journal January 2011
Potential for a biogenic influence on cloud microphysics over the ocean: a correlation study with satellite-derived data journal January 2012
Chemistry and Release of Gases from the Surface Ocean journal February 2015
Re-examination of global emerging patterns of ocean DMS concentration journal November 2011
Representation of nucleation mode microphysics in a global aerosol model with sectional microphysics journal January 2013
Global budget and radiative forcing of black carbon aerosol: Constraints from pole-to-pole (HIPPO) observations across the Pacific: GLOBAL BC BUDGET AND RADIATIVE FORCING journal January 2014
Sea-spray regulates sulfate cloud droplet activation over oceans journal April 2020
Abiotic and biotic sources influencing spring new particle formation in North East Greenland journal October 2018
Microbial Control of Sea Spray Aerosol Composition: A Tale of Two Blooms journal May 2015
The value of remote marine aerosol measurements for constraining radiative forcing uncertainty journal January 2020
Organic functional groups in the submicron aerosol at 82.5° N, 62.5° W from 2012 to 2014 journal January 2018
Laboratory simulations and parameterization of the primary marine aerosol production: THE PRIMARY MARINE AEROSOL SOURCE journal May 2003
Primary marine organic aerosol: A dichotomy of low hygroscopicity and high CCN activity: MARINE AEROSOL-CLOUD INTERACTIONS journal November 2011
Large contribution of organics to condensational growth and formation of cloud condensation nuclei (CCN) in the remote marine boundary layer journal January 2020
Influence of oceanic dimethyl sulfide emissions on cloud condensation nuclei concentrations and seasonality over the remote Southern Hemisphere oceans: A global model study journal January 2008
The physical and chemical characteristics of marine primary organic aerosol: a review journal January 2013
Connecting marine productivity to sea-spray via nanoscale biological processes: Phytoplankton Dance or Death Disco? journal October 2015
Marine Aerosols and Clouds journal January 2018
Radiative forcing by long-lived greenhouse gases: Calculations with the AER radiative transfer models journal January 2008
Observations of new particle formation in enhanced UV irradiance zones near cumulus clouds journal January 2015
Interfacial photochemistry at the ocean surface is a global source of organic vapors and aerosols journal May 2018
Marine aerosol chemistry gradients: Elucidating primary and secondary processes and fluxes: MARINE AEROSOL CHEMISTRY GRADIENTS journal April 2008
Decadal increase in Arctic dimethylsulfide emission journal September 2019
How important are future marine and shipping aerosol emissions in a warming Arctic summer and autumn? journal January 2018
Size-resolved morphological properties of the high Arctic summer aerosol during ASCOS-2008 journal January 2016
Effect of nonprecipitating clouds on the aerosol size distribution in the marine boundary layer journal February 1986
Seasonal Differences and Variability of Concentrations, Chemical Composition, and Cloud Condensation Nuclei of Marine Aerosol Over the North Atlantic journal September 2020
Marine biogenic and anthropogenic contributions to non-sea-salt sulfate in the marine boundary layer over the North Atlantic Ocean journal January 2002
An updated climatology of surface dimethlysulfide concentrations and emission fluxes in the global ocean: UPDATED DMS CLIMATOLOGY journal January 2011
UV photochemistry of carboxylic acids at the air‐sea boundary: A relevant source of glyoxal and other oxygenated VOC in the marine atmosphere journal January 2017
Investigating organic aerosol loading in the remote marine environment journal January 2011
Revised treatment of wet scavenging processes dramatically improves GEOS-Chem 12.0.0 simulations of surface nitric acid, nitrate, and ammonium over the United States journal January 2019
Iodine observed in new particle formation events in the Arctic atmosphere during ACCACIA journal January 2015
Quantifying environmental stress-induced emissions of algal isoprene and monoterpenes using laboratory measurements journal January 2015
Sea-surface dimethylsulfide (DMS) concentration from satellite data at global and regional scales journal January 2018
Biogenic, anthropogenic and sea salt sulfate size-segregated aerosols in the Arctic summer journal January 2016
Assessing the Dynamics of Organic Aerosols over the North Atlantic Ocean journal March 2017
Chemical Characterization of Isoprene- and Monoterpene-Derived Secondary Organic Aerosol Tracers in Remote Marine Aerosols over a Quarter Century journal April 2019
Low-CCN concentration air masses over the eastern North Atlantic: Seasonality, meteorology, and drivers: LOW-CCN AIR MASSES AT THE AZORES journal January 2017
Microlayer source of oxygenated volatile organic compounds in the summertime marine Arctic boundary layer journal May 2017
Contribution of sea surface carbon pool to organic matter enrichment in sea spray aerosol journal February 2014
Airborne survey of trace gases and aerosols over the Southern Baltic Sea: from clean marine boundary layer to shipping corridor effect journal December 2019
The importance of interstitial particle scavenging by cloud droplets in shaping the remote aerosol size distribution and global aerosol-climate effects journal January 2015
Organic Condensation and Particle Growth to CCN Sizes in the Summertime Marine Arctic Is Driven by Materials More Semivolatile Than at Continental Sites: Organic Condensation and Particle Growth journal October 2017
Further improvement of wet process treatments in GEOS-Chem v12.6.0: impact on global distributions of aerosols and aerosol precursors journal January 2020
Evidence for marine production of monoterpenes journal January 2008
High summertime aerosol organic functional group concentrations from marine and seabird sources at Ross Island, Antarctica, during AWARE journal January 2018
Marine aerosol, sea-salt, and the marine sulphur cycle: a short review journal January 1997
Atmospheric sulphuric acid and aerosol formation: implications from atmospheric measurements for nucleation and early growth mechanisms journal January 2006
Size-Dependent Changes in Sea Spray Aerosol Composition and Properties with Different Seawater Conditions journal May 2013
Frequent ultrafine particle formation and growth in Canadian Arctic marine and coastal environments journal January 2017
Measurements of enhanced H 2 SO 4 and 3-4 nm particles near a frontal cloud during the First Aerosol Characterization Experiment (ACE 1) journal October 2001
A large source of cloud condensation nuclei from new particle formation in the tropics journal October 2019
Global simulations of aerosol processing in clouds journal January 2008
Predicting global aerosol size distributions in general circulation models journal January 2002
Formation and growth of nucleated particles into cloud condensation nuclei: model–measurement comparison journal January 2013
Oceanic phytoplankton, atmospheric sulphur, cloud albedo and climate journal April 1987
Dimethyl sulfide and its role in aerosol formation and growth in the Arctic summer – a modelling study journal January 2019
Sensitivity of Arctic sulfate aerosol and clouds to changes in future surface seawater dimethylsulfide concentrations journal January 2019

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