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Atmosphere
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Ocean Contributions to the Marine Boundary Layer Aerosol Budget
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Ocean Contributions to the Marine Boundary Layer Aerosol Budget

A special issue of Atmosphere (ISSN 2073-4433). This special issue belongs to the section "Biosphere/Hydrosphere/Land–Atmosphere Interactions".

Deadline for manuscript submissions: closed (31 October 2018) | Viewed by 42102

Special Issue Editors

Prof. Dr. Nicholas Meskhidze

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Guest Editor
Department of Marine, Earth and Atmospheric Sciences, North Carolina State University, Raleigh, NC 27695, USA
Interests: measurements of vertical turbulent fluxes of size-selected particles using Eddy Covariance and Relaxed Eddy Accumulation techniques; application of active remotely sensing (i.e., High Spectral Resolution Lidar, HSRL) for deriving aerosol chemical composition and direct radiative forcing; Improved characterization of air-sea transport of bioaccessible iron through novel laboratory techniques and 3D chemistry transport models
Dr. Matthew Salter

E-Mail Website
Guest Editor
Department of Environmental Science and Analytical Chemistry, Faculty of Science, Stockholms Universitet, Stockholm, Sweden
Interests: sea spay aerosol; air–sea gas exchange; air–sea interaction; sea surface microlayer
Dr. Karine Sellegri

E-Mail
Guest Editor
Laboratoire de Météorologie Physique, Universite Blaise Pascal, Clermont-Ferrand, France
Interests: experimental; sea–air exchanges; aerosol natural emissions; nucleation; aerosol hygroscopic properties; aerosol–cloud interactions
Dr. Scott Elliott

E-Mail
Guest Editor
Los Alamos National Laboratory, Los Alamos, USA
Interests: sea–air transfer; trace gases; dimethyl sulfide; dissolved organic carbon; marine biomacromolecules; natural surfactants; micro-layer adsorption; wave breaking and bubbles; primary organic aerosol; global surface tension and surface pressure; momentum and heat fluxes

Special Issue Information

Dear Colleagues,

Recent studies have shown that an accurate representation of natural background aerosols is critical for improved assessment of direct and indirect anthropogenic aerosol forcing. The reduction of the uncertainties over the representation of natural aerosols in climate models requires improved quantification of number, size distribution, chemical composition, and hygroscopic properties of aerosol in the marine boundary layer (MBL). This Special Issue invites contributions from modeling, field, laboratory, and satellite studies related to 1) production of sea-spray aerosol (SSA) and ocean-derived biogenic volatile organic compounds (VOCs), 2) characterization of size-resolved chemical composition of aerosols in the MBL, and 3) assessments for the contribution of ocean-derived primary and secondary aerosols to the MBL cloud condensation nuclei (CCN) and ice nucleating particle (INP) number budget.

This Special Issue is motivated by our perceived need to provide a platform for current discussions regarding the oceanic contribution to the MBL aerosol, CCN, and INP number concentration over different parts of the oceans. Global models estimate the production of SSA using wind speed-dependent flux parameterizations, often based on a whitecap method developed under laboratory settings. Ambient studies infer effective SSA production from the ocean using micrometeorological techniques such as the eddy covariance and the gradient method that measure total sub-micron or size-selected particle fluxes in the lowest portion of the MBL. Despite its importance, to this day the size- and composition-dependent production flux of primary SSA particles and its dependence on environmental variables remains poorly characterized. Likewise, oceanic emission rates of biogenic (VOCs) (e.g., dimethyl sulfide (DMS), isoprene, monoterpenes, and iodocarbons) leading to the secondary aerosol production in the MBL are not well constrained. The dependence of the emissions rates on types of phytoplankton and bacteria, as well as environmental parameters such as wind speed, light, and nutrients is not well quantified. Current models also do not fully address marine emission and their relationships with eco-physiological factors, evolutionary drivers, and global consequences. As a result, contribution of oceanic sources to the MBL aerosol, CCN, and INP number budgets remain poorly defined.

Prof. Dr. Nicholas  Meskhidze
Dr. Matthew Salter
Dr. Karine Sellegri
Dr. Scott  Elliott
Guest Editors

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All submissions that pass pre-check are peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 100 words) can be sent to the Editorial Office for announcement on this website.

Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Atmosphere is an international peer-reviewed open access monthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 2400 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

  • sea-spray aerosol

  • cloud condensation nuclei

  • ice nucleating particles

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Published Papers (8 papers)

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Editorial

Jump to: Research, Other

3 pages, 157 KiB  
Editorial
Ocean Contributions to the Marine Boundary Layer Aerosol Budget
by Nicholas Meskhidze, Matthew Salter, Karine Sellegri and Scott Elliott
Atmosphere 2019, 10(2), 98; https://doi.org/10.3390/atmos10020098 - 23 Feb 2019
Cited by 2 | Viewed by 2883
Abstract
Projections of future climate remain an important scientific goal for much of the Earth science community [...] Full article
(This article belongs to the Special Issue Ocean Contributions to the Marine Boundary Layer Aerosol Budget)

Research

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16 pages, 1564 KiB  
Article
Collapse Mechanisms of Nascent and Aged Sea Spray Aerosol Proxy Films
by Kimberly A. Carter-Fenk and Heather C. Allen
Atmosphere 2018, 9(12), 503; https://doi.org/10.3390/atmos9120503 - 18 Dec 2018
Cited by 16 | Viewed by 6244
Abstract
Sea spray aerosol (SSA) is highly enriched in marine-derived organic compounds during seasons of high biological productivity, and saturated fatty acids comprise one of the most abundant classes of molecules. Fatty acids and other organic compounds form a film on SSA surfaces, and [...] Read more.
Sea spray aerosol (SSA) is highly enriched in marine-derived organic compounds during seasons of high biological productivity, and saturated fatty acids comprise one of the most abundant classes of molecules. Fatty acids and other organic compounds form a film on SSA surfaces, and SSA particle surface-area-to-volume ratios are altered during aging in the marine boundary layer (MBL). To understand SSA surface organization and its role during dynamic atmospheric conditions, an SSA proxy fatty acid film and its individual components stearic acid (SA), palmitic acid (PA), and myristic acid (MA) are studied separately using surface pressure–area ( Π − A ) isotherms and Brewster angle microscopy (BAM). The films were spread on an aqueous NaCl subphase at pH 8.2, 5.6, and 2.0 to mimic nascent to aged SSA aqueous core composition in the MBL, respectively. We show that the individual fatty acid behavior differs from that of the SSA proxy film, and at nascent SSA pH the mixture yields a monolayer with intermediate rigidity that folds upon film compression to the collapse state. Acidification causes the SSA proxy film to become more rigid and form 3D nuclei. Our results reveal film morphology alterations, which are related to SSA reflectivity, throughout various stages of SSA aging and provide a better understanding of SSA impacts on climate. Full article
(This article belongs to the Special Issue Ocean Contributions to the Marine Boundary Layer Aerosol Budget)
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17 pages, 1872 KiB  
Article
The Impact of Divalent Cations on the Enrichment of Soluble Saccharides in Primary Sea Spray Aerosol
by Steven R. Schill, Susannah M. Burrows, Elias S. Hasenecz, Elizabeth A. Stone and Timothy H. Bertram
Atmosphere 2018, 9(12), 476; https://doi.org/10.3390/atmos9120476 - 4 Dec 2018
Cited by 19 | Viewed by 5799
Abstract
Field measurements have shown that sub-micrometer sea spray aerosol (SSA) is significantly enriched in organic material, of which a large fraction has been attributed to soluble saccharides. Existing mechanistic models of SSA production struggle to replicate the observed enhancement of soluble organic material. [...] Read more.
Field measurements have shown that sub-micrometer sea spray aerosol (SSA) is significantly enriched in organic material, of which a large fraction has been attributed to soluble saccharides. Existing mechanistic models of SSA production struggle to replicate the observed enhancement of soluble organic material. Here, we assess the role for divalent cation mediated co-adsorption of charged surfactants and saccharides in the enrichment of soluble organic material in SSA. Using measurements of particle supersaturated hygroscopicity, we calculate organic volume fractions for molecular mimics of SSA generated from a Marine Aerosol Reference Tank. Large enhancements in SSA organic volume fractions (Xorg > 0.2) were observed for 50 nm dry diameter (dp) particles in experiments where cooperative ionic interactions were favorable (e.g., palmitic acid, Mg2+, and glucuronic acid) at seawater total organic carbon concentrations (<1.15 mM C) and ocean pH. Significantly smaller SSA organic volume fractions (Xorg < 1.5 × 10−3) were derived from direct measurements of soluble saccharide concentrations in collected SSA with dry diameters <250 nm, suggesting that organic enrichment is strongly size dependent. The results presented here indicate that divalent cation mediated co-adsorption of soluble organics to insoluble surfactants at the ocean surface may contribute to the enrichment of soluble saccharides in SSA. The extent to which this mechanism explains the observed enhancement of saccharides in nascent SSA depends strongly on the concentration, speciation, and charge of surfactants and saccharides in the sea surface microlayer. Full article
(This article belongs to the Special Issue Ocean Contributions to the Marine Boundary Layer Aerosol Budget)
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32 pages, 3552 KiB  
Article
Does Marine Surface Tension Have Global Biogeography? Addition for the OCEANFILMS Package
by Scott Elliott, Susannah Burrows, Philip Cameron-Smith, Forrest Hoffman, Elizabeth Hunke, Nicole Jeffery, Yina Liu, Mathew Maltrud, Zachary Menzo, Oluwaseun Ogunro, Luke Van Roekel, Shanlin Wang, Michael Brunke, Meibing Jin, Robert Letscher, Nicholas Meskhidze, Lynn Russell, Isla Simpson, Dale Stokes and Oliver Wingenter
Atmosphere 2018, 9(6), 216; https://doi.org/10.3390/atmos9060216 - 4 Jun 2018
Cited by 10 | Viewed by 6470
Abstract
We apply principles of Gibbs phase plane chemistry across the entire ocean-atmosphere interface to investigate aerosol generation and geophysical transfer issues. Marine surface tension differences comprise a tangential pressure field controlling trace gas fluxes, primary organic inputs, and sea spray salt injections, in [...] Read more.
We apply principles of Gibbs phase plane chemistry across the entire ocean-atmosphere interface to investigate aerosol generation and geophysical transfer issues. Marine surface tension differences comprise a tangential pressure field controlling trace gas fluxes, primary organic inputs, and sea spray salt injections, in addition to heat and momentum fluxes. Mapping follows from the organic microlayer composition, now represented in ocean system models. Organic functional variations drive the microforcing, leading to (1) reduced turbulence and (by extension) laminar gas-energy diffusion; plus (2) altered bubble film mass emission into the boundary layer. Interfacial chemical behaviors are, therefore, closely reviewed as the background. We focus on phase transitions among two dimensional “solid, liquid, and gaseous” states serving as elasticity indicators. From the pool of dissolved organic carbon (DOC) only proteins and lipids appear to occupy significant atmospheric interfacial areas. The literature suggests albumin and stearic acid as the best proxies, and we distribute them through ecodynamic simulation. Consensus bulk distributions are obtained to control their adsorptive equilibria. We devise parameterizations for both the planar free energy and equation of state, relating excess coverage to the surface pressure and its modulus. Constant settings for the molecular surrogates are drawn from laboratory study and successfully reproduce surfactant solid-to-gas occurrence in compression experiments. Since DOC functionality measurements are rare, we group them into super-ecological province tables to verify aqueous concentration estimates. Outputs are then fed into a coverage, tension, elasticity code. The resulting two dimensional pressure contours cross a critical range for the regulation of precursor piston velocity, bubble breakage, and primary aerosol sources plus ripple damping. Concepts extend the water-air adsorption theory currently embodied in our OCEANFILMS aerosol emissions package, and the two approaches could be inserted into Earth System Models together. Uncertainties in the logic include kinetic and thermochemical factors operating at multiple scales. Full article
(This article belongs to the Special Issue Ocean Contributions to the Marine Boundary Layer Aerosol Budget)
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21 pages, 2766 KiB  
Article
Evaluating Uncertainties in Marine Biogeochemical Models: Benchmarking Aerosol Precursors
by Oluwaseun O. Ogunro, Scott M. Elliott, Oliver W. Wingenter, Clara Deal, Weiwei Fu, Nathan Collier and Forrest M. Hoffman
Atmosphere 2018, 9(5), 184; https://doi.org/10.3390/atmos9050184 - 12 May 2018
Cited by 4 | Viewed by 5546
Abstract
The effort to accurately estimate global radiative forcing has long been hampered by a degree of uncertainty in the tropospheric aerosol contribution. Reducing uncertainty in natural aerosol processes, the baseline of the aerosol budget, thus becomes a fundamental task. The appropriate representation of [...] Read more.
The effort to accurately estimate global radiative forcing has long been hampered by a degree of uncertainty in the tropospheric aerosol contribution. Reducing uncertainty in natural aerosol processes, the baseline of the aerosol budget, thus becomes a fundamental task. The appropriate representation of aerosols in the marine boundary layer (MBL) is essential to reduce uncertainty and provide reliable information on offsets to global warming. We developed an International Ocean Model Benchmarking package to assess marine biogeochemical process representations in Earth System Models (ESMs), and the package was employed to evaluate surface ocean concentrations and the sea–air fluxes of dimethylsulfide (DMS). Model performances were scored based on how well they captured the distribution and variability contained in high-quality observational datasets. Results show that model-data biases increased as DMS enters the MBL, but unfortunately over three-quarters of the models participating in the fifth Coupled Model Intercomparison Project (CMIP5) did not have a dynamic representation of DMS. When it is present, models tend to over-predict sea surface concentrations in the productive region of the eastern tropical Pacific by almost a factor of two, and the sea–air fluxes by a factor of three. Systematic model-data benchmarking as described here will help to identify such deficiencies and subsequently lead to improved subgrid-scale parameterizations and ESM development. Full article
(This article belongs to the Special Issue Ocean Contributions to the Marine Boundary Layer Aerosol Budget)
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21 pages, 2460 KiB  
Article
Climate Change Impacts on Natural Sulfur Production: Ocean Acidification and Community Shifts
by Zachary M. Menzo, Scott Elliott, Corinne A. Hartin, Forrest M. Hoffman and Shanlin Wang
Atmosphere 2018, 9(5), 167; https://doi.org/10.3390/atmos9050167 - 1 May 2018
Cited by 8 | Viewed by 5527
Abstract
Utilizing the reduced-complexity model Hector, a regional scale analysis was conducted quantifying the possible effects climate change may have on dimethyl sulfide (DMS) emissions within the oceans. The investigation began with a review of the sulfur cycle in modern Earth system models. We [...] Read more.
Utilizing the reduced-complexity model Hector, a regional scale analysis was conducted quantifying the possible effects climate change may have on dimethyl sulfide (DMS) emissions within the oceans. The investigation began with a review of the sulfur cycle in modern Earth system models. We then expanded the biogeochemical representation within Hector to include a natural ocean component while accounting for acidification and planktonic community shifts. The report presents results from both a latitudinal and a global perspective. This new approach highlights disparate outcomes which have been inadequately characterized via planetary averages in past publications. Our findings suggest that natural sulfur emissions (ESN) may exert a forcing up to 4 times that of the CO2 marine feedback, 0.62 and 0.15 Wm−2, respectively, and reverse the radiative forcing sign in low latitudes. Additionally, sensitivity tests were conducted to demonstrate the need for further examination of the DMS loop. Ultimately, the present work attempts to include dynamic ESN within reduced-complexity simulations of the sulfur cycle, illustrating its impact on the global radiative budget. Full article
(This article belongs to the Special Issue Ocean Contributions to the Marine Boundary Layer Aerosol Budget)
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19 pages, 5878 KiB  
Article
Effect of Wind Speed on Moderate Resolution Imaging Spectroradiometer (MODIS) Aerosol Optical Depth over the North Pacific
by Lena Merkulova, Eyal Freud, E. Monica Mårtensson, E. Douglas Nilsson and Paul Glantz
Atmosphere 2018, 9(2), 60; https://doi.org/10.3390/atmos9020060 - 9 Feb 2018
Cited by 9 | Viewed by 5192
Abstract
The surface-wind speed influences on aerosol optical depth (AOD), derived from the Moderate Resolution Imaging Spectroradiometer (MODIS) Aqua daily observations over the central North Pacific during the period 2003–2016, have been investigated in this study. The cloud coverage is relatively low over the [...] Read more.
The surface-wind speed influences on aerosol optical depth (AOD), derived from the Moderate Resolution Imaging Spectroradiometer (MODIS) Aqua daily observations over the central North Pacific during the period 2003–2016, have been investigated in this study. The cloud coverage is relatively low over the present investigation area compared to other marine areas, which favors AOD derived from passive remote sensing from space. In this study, we have combined MODIS AOD with 2 m wind speed (U2m) on a satellite-pixel basis, which has been interpolated from National Centers for Environmental Prediction (NCEP) reanalysis. In addition, daily averaged AOD derived from Aerosol Robotic Network (AERONET) measurements in the free-troposphere at the Mauna Loa Observatory (3397 m above sea level), Hawaii, was subtracted from the MODIS column AOD values. The latter was to reduce the contribution of aerosols above the planetary boundary layer. This study shows relatively strong power-law relationships between MODIS mean AOD and surface-wind speed for marine background conditions in summer, fall and winter of the current period. However, previous established relationships between AOD and surface-wind speed deviate substantially. Even so, for similar marine conditions the present relationship agrees reasonable well with a power-law relationship derived for north-east Atlantic conditions. The present MODIS retrievals of AOD in the marine atmosphere agree reasonably well with ground-based remote sensing of AOD. Full article
(This article belongs to the Special Issue Ocean Contributions to the Marine Boundary Layer Aerosol Budget)
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Other

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15 pages, 6462 KiB  
Technical Note
Web Strategy to Convey Marine Biogeochemical Feedback Concepts to the Policy Community: Aerosol and Sea Ice
by Zachary M. Menzo
Atmosphere 2018, 9(1), 22; https://doi.org/10.3390/atmos9010022 - 16 Jan 2018
Cited by 2 | Viewed by 3680
Abstract
Limited understanding of the climate system imposes upon policy makers an intimate reliance on results from Earth System Models (ESMs). However, climate simulations are necessarily incomplete since many strong channels through planetary scale biology and geochemistry remain too complex or poorly comprehended to [...] Read more.
Limited understanding of the climate system imposes upon policy makers an intimate reliance on results from Earth System Models (ESMs). However, climate simulations are necessarily incomplete since many strong channels through planetary scale biology and geochemistry remain too complex or poorly comprehended to include. This paper presents and describes an interactive, public domain website detailing the role of two marine biogeochemical (mBGC) feedback loops currently excluded from many ESMs (www.marinefeedbacks.com). Every page on the website includes images or videos to foster engagement with its technically challenging content. Simultaneously, fundamentals of the natural science involved are reinforced. The site includes subsections of the following nature; background information, executive summaries for each feedback type, detailed descriptions of the chemical mechanisms, climate change impact, and recommendations for future research. The information provided is firmly grounded in the technical literature but is designed specifically for accessibility to non-scientists. Particular targets for the material are the next-generation of decision makers and those framing the international climate agenda. It is hoped that a site with tailored pedagogical value may contribute to well informed policy formulation and legislation. Full article
(This article belongs to the Special Issue Ocean Contributions to the Marine Boundary Layer Aerosol Budget)
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