scholarly journals Mediterranean nascent sea spray organic aerosol and relationships with seawater biogeochemistry

2021 ◽  
Vol 21 (13) ◽  
pp. 10625-10641
Author(s):  
Evelyn Freney ◽  
Karine Sellegri ◽  
Alessia Nicosia ◽  
Leah R. Williams ◽  
Matteo Rinaldi ◽  
...  
Keyword(s):  
Organic Carbon ◽  
Particulate Organic Carbon ◽  
Time Resolution ◽  
Ambient Air ◽  
Organic Aerosol ◽  
Daily Basis ◽  
Sea Spray ◽  
Surface Seawater ◽  
Cell Abundance ◽  
Sea Spray Aerosol

Abstract. The organic mass fraction from sea spray aerosol (SSA) is currently a subject of intense research. The majority of this research is dedicated to measurements in ambient air. However a number of studies have recently started to focus on nascent sea spray aerosol. This work presents measurements collected during a 5-week cruise in May and June 2017 in the central and western Mediterranean Sea, an oligotrophic marine region with low phytoplankton biomass. Surface seawater was continuously pumped into a bubble-bursting apparatus to generate nascent sea spray aerosol. Size distributions were measured with a differential mobility particle sizer (DMPS). Chemical characterization of the submicron aerosol was performed with a time-of-flight aerosol chemical speciation monitor (ToF-ACSM) operating with 10 min time resolution and with filter-based chemical analysis on a daily basis. Using positive matrix factorization analysis, the ToF-ACSM non-refractory organic matter (OMNR) was separated into four different organic aerosol types, identified as primary OA (POANR), oxidized OA (OOANR), methanesulfonic acid type OA (MSA-OANR), and mixed OA (MOANR). In parallel, surface seawater biogeochemical properties were monitored providing information on phytoplankton cell abundance and seawater particulate organic carbon (1 h time resolution) and seawater surface microlayer (SML) dissolved organic carbon (DOC) (on a daily basis). Statistically robust correlations (for n>500) were found between MOANR and nanophytoplankton cell abundance, as well as between POANR, OOANR, and particulate organic carbon (POC). Parameterizations of the contributions of different types of organics to the submicron nascent sea spray aerosol are proposed as a function of the seawater biogeochemical properties for use in models.

scholarly journals Mediterranean nascent sea spray organic aerosol and relationships with seawater biogeochemistry

2020 ◽  
Author(s):  
Evelyn Freney ◽  
Karine Sellegri ◽  
Alessia Nicosia ◽  
Jonathan T. Trueblood ◽  
Matteo Rinaldi ◽  
...  
Keyword(s):  
Organic Carbon ◽  
Particulate Organic Carbon ◽  
Time Resolution ◽  
Daily Basis ◽  
Sea Spray ◽  
Surface Seawater ◽  
Organic Mass ◽  
Cell Abundance ◽  
Phytoplankton Cell ◽  
Sea Spray Aerosol

Abstract. The organic mass fraction from sea spray aerosol (SSA) is currently a subject of intense research. The majority of this research is dedicated to measurements in ambient air, although recently a small number of studies have additionally focused on nascent sea spray aerosol. This work presents measurements collected during a five-week cruise in May and June 2017 in the central and western Mediterranean Sea, an oligotrophic marine region with low phytoplankton biomass. Surface seawater was continuously pumped into a bubble bursting apparatus to generate nascent sea spray aerosol. Size distributions were measured with a differential mobility particle sizer (DMPS). Chemical characterization of the submicron aerosol was performed with a time of flight aerosol chemical speciation monitor (ToF-ACSM) operating with a 15-minute time resolution, and with filter-based chemical analysis on a daily basis. Using a positive matrix factorization analysis, the ToF-ACSM non-refractory organic matter (OMNR) was separated into four different organic aerosols types which were identified as primary OA (POANR), oxidized OA (OOANR), a methanesulfonic acid type OA (MSA-OANR) and a mixed OA (MOANR). In parallel, surface seawater biogeochemical properties were monitored providing information on phytoplankton cell abundance and seawater particulate organic carbon (one-hour time resolution), and seawater surface microlayer (SML) dissolved organic carbon (DOC) (on a daily basis). Statistically robust correlations (for n > 500) were found between MOANR and nano phytoplankton cell abundance, as well as between POANR, OOANR, and particulate organic carbon (POC). Filter-based analysis of the submicron SSA showed that the non-refractory organic mass represented only 13 ± 3 % of the total organic mass, which represents 22 ± 6 % of the total sea spray mass. Parameterizations of the contributions of different types of organics to the submicron nascent sea spray aerosol are proposed as a function of the seawater biogeochemical properties for use in models.

scholarly journals Effect of primary organic sea spray emissions on cloud condensation nuclei concentrations

2012 ◽  
Vol 12 (1) ◽  
pp. 89-101 ◽  
Author(s):  
D. M. Westervelt ◽  
R. H. Moore ◽  
A. Nenes ◽  
P. J. Adams
Keyword(s):  
Surface Tension ◽  
Southern Ocean ◽  
Source Function ◽  
Cloud Condensation Nuclei ◽  
Organic Aerosol ◽  
Sea Salt ◽  
Sea Spray ◽  
Aerosol Emission ◽  
Sea Spray Aerosol ◽  
Surfactant Effects

Abstract. This work estimates the primary marine organic aerosol global emission source and its impact on cloud condensation nuclei (CCN) concentrations by implementing an organic sea spray source function into a series of global aerosol simulations. The source function assumes that a fraction of the sea spray emissions, depending on the local chlorophyll concentration, is organic matter in place of sea salt. Effect on CCN concentrations (at 0.2% supersaturation) is modeled using the Two-Moment Aerosol Sectional (TOMAS) microphysics algorithm coupled to the GISS II-prime general circulation model. The presence of organics affects CCN activity in competing ways: by reducing the amount of solute available in the particle and decreasing surface tension of CCN. To model surfactant effects, surface tension depression data from seawater samples taken near the Georgia coast were applied as a function of carbon concentrations. A global marine organic aerosol emission rate of 17.7 Tg C yr−1 is estimated from the simulations. Marine organics exert a localized influence on CCN(0.2%) concentrations, decreasing regional concentrations by no more than 5% and by less than 0.5% over most of the globe, assuming direct replacement of sea salt aerosol with organic aerosol. The decrease in CCN concentrations results from the fact that the decrease in particle solute concentration outweighs the organic surfactant effects. The low sensitivity of CCN(0.2%) to the marine organic emissions is likely due to the small compositional changes: the mass fraction of OA in accumulation mode aerosol increases by only ~15% in a biologically active region of the Southern Ocean. To test the sensitivity to uncertainty in the sea spray emissions process, we relax the assumption that sea spray aerosol number and mass remain fixed and instead can add to sea spray emissions rather than replace existing sea salt. In these simulations, we find that marine organic aerosol can increase CCN by up to 50% in the Southern Ocean and 3.7% globally during the austral summer. This vast difference in CCN impact highlights the need for further observational exploration of the sea spray aerosol emission process as well as evaluation and development of model parameterizations.

scholarly journals Wind speed dependent size-resolved parameterization for the organic mass fraction of sea spray aerosol

2011 ◽  
Vol 11 (16) ◽  
pp. 8777-8790 ◽  
Author(s):  
B. Gantt ◽  
N. Meskhidze ◽  
M. C. Facchini ◽  
M. Rinaldi ◽  
D. Ceburnis ◽  
...  
Keyword(s):  
Chemical Composition ◽  
Wind Speed ◽  
Organic Carbon ◽  
Mass Fraction ◽  
Surface Wind ◽  
Surface Wind Speed ◽  
Sea Spray ◽  
Organic Mass ◽  
Chl A ◽  
Sea Spray Aerosol

Abstract. For oceans to be a significant source of primary organic aerosol (POA), sea spray aerosol (SSA) must be highly enriched with organics relative to the bulk seawater. We propose that organic enrichment at the air-sea interface, chemical composition of seawater, and the aerosol size are three main parameters controlling the organic mass fraction of sea spray aerosol (OMSSA). To test this hypothesis, we developed a new marine POA emission function based on a conceptual relationship between the organic enrichment at the air-sea interface and surface wind speed. The resulting parameterization is explored using aerosol chemical composition and surface wind speed from Atlantic and Pacific coastal stations, and satellite-derived ocean concentrations of chlorophyll-a, dissolved organic carbon, and particulate organic carbon. Of all the parameters examined, a multi-variable logistic regression revealed that the combination of 10 m wind speed and surface chlorophyll-a concentration ([Chl-a]) are the most consistent predictors of OMSSA. This relationship, combined with the published aerosol size dependence of OMSSA, resulted in a new parameterization for the organic mass fraction of SSA. Global emissions of marine POA are investigated here by applying this newly-developed relationship to existing sea spray emission functions, satellite-derived [Chl-a], and modeled 10 m winds. Analysis of model simulations shows that global annual submicron marine organic emission associated with sea spray is estimated to be from 2.8 to 5.6 Tg C yr−1. This study provides additional evidence that marine primary organic aerosols are a globally significant source of organics in the atmosphere.

Studies on Phytoplankton and Particulate Organic Carbon in the Southern Ocean

2011 ◽  
Vol 137 ◽  
pp. 344-352
Author(s):  
Gen Hai Zhu ◽  
Yan Lan Liu ◽  
Li Hong Chen ◽  
Pei Song Yu ◽  
Mao Jin ◽  
...  
Keyword(s):  
Organic Carbon ◽  
Southern Ocean ◽  
Particulate Organic Carbon ◽  
Euphotic Zone ◽  
Study Data ◽  
Phytoplankton Abundance ◽  
Average Cell ◽  
Chl A ◽  
Cell Abundance ◽  
Phytoplankton Cell

Using China Southern Ocean’s study data collected from 1989 to 2009 year, this paper analyzed the related characteristics between phytoplankton abundance, Ch1 a concentrations and particulate organic carbon. The average cell abundance of Southern Ocean phytoplankton was 7.38×104 cells/dm3. The dominant species of Southern Ocean phytoplankton were Fragilariopsis kerguelensis, Fragilariopsis curta, Pseudo-nitzschia lineola, Eucampia antarctica, Thalassiosira antarctica and Corethron criophilum and son on. In Prydz Bay of the Southern Ocean, the contribution of phytoplankton cell abundance and phytoplankton carbon toward particulate organic carbon were higher than that in the Northern Gulf Ocean Area. In the upper layer of euphotic zone, the contribution of phytoplankton abundance and phytoplankton carbon toward particulate organic carbon were higher than that in the deep water district. Through analysis of regressive statistics, phytoplankton cell abundance (y) and particulate organic carbon (POC) and chlorophyll a (Chl a) were a remarkable positive correlation.

scholarly journals Secondary sulfate is internally mixed with sea spray aerosol and organic aerosol in the winter Arctic

2018 ◽  
Vol 18 (6) ◽  
pp. 3937-3949 ◽  
Author(s):  
Rachel M. Kirpes ◽  
Amy L. Bondy ◽  
Daniel Bonanno ◽  
Ryan C. Moffet ◽  
Bingbing Wang ◽  
...  
Keyword(s):  
Chemical Composition ◽  
Organic Carbon ◽  
Pollutant Emissions ◽  
Cloud Formation ◽  
Sea Spray ◽  
X Ray ◽  
Atmospheric Processing ◽  
Arctic Aerosol ◽  
Scanning Transmission ◽  
Sea Spray Aerosol

Abstract. Few measurements of aerosol chemical composition have been made during the winter–spring transition (following polar sunrise) to constrain Arctic aerosol–cloud–climate feedbacks. Herein, we report the first measurements of individual particle chemical composition near Utqiaġvik (Barrow), Alaska, in winter (seven sample days in January and February 2014). Individual particles were analyzed by computer-controlled scanning electron microscopy with energy dispersive X-ray spectroscopy (CCSEM-EDX, 24 847 particles), Raman microspectroscopy (300 particles), and scanning transmission X-ray microscopy with near-edge X-ray absorption fine structure spectroscopy (STXM-NEXAFS, 290 particles). Sea spray aerosol (SSA) was observed in all samples, with fresh and aged SSA comprising 99 %, by number, of 2.5–7.5 µm diameter particles, 65–95 % from 0.5–2.5 µm, and 50–60 % from 0.1–0.5 µm, indicating SSA is the dominant contributor to accumulation and coarse-mode aerosol during the winter. The aged SSA particles were characterized by reduced chlorine content with 94 %, by number, internally mixed with secondary sulfate (39 %, by number, internally mixed with both nitrate and sulfate), indicative of multiphase aging reactions during transport. There was a large number fraction (40 % of 1.0–4.0 µm diameter particles) of aged SSA during periods when particles were transported from near Prudhoe Bay, consistent with pollutant emissions from the oil fields participating in atmospheric processing of aerosol particles. Organic carbon and sulfate particles were observed in all samples and comprised 40–50 %, by number, of 0.1–0.4 µm diameter particles, indicative of Arctic haze influence. Soot was internally mixed with organic and sulfate components. All sulfate was mixed with organic carbon or SSA particles. Therefore, aerosol sources in the Alaskan Arctic and resulting aerosol chemical mixing states need to be considered when predicting aerosol climate effects, particularly cloud formation, in the winter Arctic.

scholarly journals Model evaluation of marine primary organic aerosol emission schemes

2012 ◽  
Vol 12 (18) ◽  
pp. 8553-8566 ◽  
Author(s):  
B. Gantt ◽  
M. S. Johnson ◽  
N. Meskhidze ◽  
J. Sciare ◽  
J. Ovadnevaite ◽  
...  
Keyword(s):  
Model Comparison ◽  
Transport Model ◽  
Organic Aerosol ◽  
Sea Spray ◽  
Mean Values ◽  
Chl A ◽  
Aerosol Mass ◽  
Aerosol Mass Concentration ◽  
Aerosol Emission ◽  
Sea Spray Aerosol

Abstract. In this study, several marine primary organic aerosol (POA) emission schemes have been evaluated using the GEOS-Chem chemical transport model in order to provide guidance for their implementation in air quality and climate models. These emission schemes, based on varying dependencies of chlorophyll a concentration ([chl a]) and 10 m wind speed (U10), have large differences in their magnitude, spatial distribution, and seasonality. Model comparison with weekly and monthly mean values of the organic aerosol mass concentration at two coastal sites shows that the source function exclusively related to [chl a] does a better job replicating surface observations. Sensitivity simulations in which the negative U10 and positive [chl a] dependence of the organic mass fraction of sea spray aerosol are enhanced show improved prediction of the seasonality of the marine POA concentrations. A top-down estimate of submicron marine POA emissions based on the parameterization that compares best to the observed weekly and monthly mean values of marine organic aerosol surface concentrations has a global average emission rate of 6.3 Tg yr−1. Evaluation of existing marine POA source functions against a case study during which marine POA contributed the major fraction of submicron aerosol mass shows that none of the existing parameterizations are able to reproduce the hourly-averaged observations. Our calculations suggest that in order to capture episodic events and short-term variability in submicron marine POA concentration over the ocean, new source functions need to be developed that are grounded in the physical processes unique to the organic fraction of sea spray aerosol.

scholarly journals North Atlantic marine organic aerosol characterized by novel offline thermal desorption mass spectrometry: polysaccharides, recalcitrant material, and secondary organics

2020 ◽  
Vol 20 (24) ◽  
pp. 16007-16022
Author(s):  
Michael J. Lawler ◽  
Savannah L. Lewis ◽  
Lynn M. Russell ◽  
Patricia K. Quinn ◽  
Timothy S. Bates ◽  
...  
Keyword(s):  
Mass Spectrometry ◽  
Organic Compounds ◽  
Thermal Desorption ◽  
North Atlantic ◽  
Size Fraction ◽  
Ambient Air ◽  
Organic Aerosol ◽  
Sea Spray ◽  
Ionization Mass ◽  
Marine Aerosol

Abstract. The composition of organic compounds in marine aerosols and the relative contributions of primary and secondary organic compounds remain uncertain. We report results from a novel approach to characterize and quantify organic components of the marine aerosol. Size-segregated discrete aerosol filter samples were collected at sea in the North Atlantic from both ambient aerosol and artificially generated primary sea spray over four cruises timed to capture the seasonal phytoplankton bloom dynamics. Samples were analyzed by Fourier transform infrared spectroscopy (FTIR), extracted into water, and analyzed by offline thermal desorption chemical ionization mass spectrometry (TDCIMS) and ion chromatography (IC). A positive matrix factorization (PMF) analysis identified several characteristic aerosol components in the TDCIMS mass spectra. Among these is a polysaccharide factor representing about 10 %–30 % of the submicron organic aerosol mass. Aerosol polysaccharide : sodium mass ratios were consistently higher in ambient air than in the artificially generated sea spray, and we hypothesize that this results from more rapid wet deposition of sodium-rich aerosol. An unquantified recalcitrant factor of highly thermally stable organics showed significant correlation with FTIR-measured alcohol groups, consistently the main organic functional group associated with sea spray aerosol. We hypothesize that this factor represents recalcitrant dissolved organic matter (DOM) in seawater and that by extension alcohol functional groups identified in marine aerosol may more typically represent recalcitrant DOM rather than biogenic saccharide-like material, contrary to inferences made in previous studies. The recalcitrant factor showed little seasonal variability in its contribution to primary marine aerosol. The relative contribution of polysaccharides was highest in late spring and summer in the smallest particle size fraction characterized (<180 nm).

scholarly journals A physically based framework for modeling the organic fractionation of sea spray aerosol from bubble film Langmuir equilibria

2014 ◽  
Vol 14 (24) ◽  
pp. 13601-13629 ◽  
Author(s):  
S. M. Burrows ◽  
O. Ogunro ◽  
A. A. Frossard ◽  
L. M. Russell ◽  
P. J. Rasch ◽  
...  
Keyword(s):  
Organic Matter ◽  
Organic Carbon ◽  
Dissolved Organic Carbon ◽  
Chlorophyll A ◽  
Sea Spray ◽  
Model Parameters ◽  
Model Calculations ◽  
Langmuir Adsorption ◽  
Marine Organic Matter ◽  
Sea Spray Aerosol

Abstract. The presence of a large fraction of organic matter in primary sea spray aerosol (SSA) can strongly affect its cloud condensation nuclei activity and interactions with marine clouds. Global climate models require new parameterizations of the SSA composition in order to improve the representation of these processes. Existing proposals for such a parameterization use remotely sensed chlorophyll a concentrations as a proxy for the biogenic contribution to the aerosol. However, both observations and theoretical considerations suggest that existing relationships with chlorophyll a, derived from observations at only a few locations, may not be representative for all ocean regions. We introduce a novel framework for parameterizing the fractionation of marine organic matter into SSA based on a competitive Langmuir adsorption equilibrium at bubble surfaces. Marine organic matter is partitioned into classes with differing molecular weights, surface excesses, and Langmuir adsorption parameters. The classes include a lipid-like mixture associated with labile dissolved organic carbon (DOC), a polysaccharide-like mixture associated primarily with semilabile DOC, a protein-like mixture with concentrations intermediate between lipids and polysaccharides, a processed mixture associated with recalcitrant surface DOC, and a deep abyssal humic-like mixture. Box model calculations have been performed for several cases of organic adsorption to illustrate the underlying concepts. We then apply the framework to output from a global marine biogeochemistry model, by partitioning total dissolved organic carbon into several classes of macromolecules. Each class is represented by model compounds with physical and chemical properties based on existing laboratory data. This allows us to globally map the predicted organic mass fraction of the nascent submicron sea spray aerosol. Predicted relationships between chlorophyll a and organic fraction are similar to existing empirical parameterizations, but can vary between biologically productive and nonproductive regions, and seasonally within a given region. Major uncertainties include the bubble film thickness at bursting, and the variability of organic surfactant activity in the ocean, which is poorly constrained. In addition, polysaccharides may enter the aerosol more efficiently than Langmuir adsorption would suggest. Potential mechanisms for enrichment of polysaccharides in sea spray include the formation of marine colloidal particles that may be more efficiently swept up by rising bubbles, and cooperative adsorption of polysaccharides with proteins or lipids. These processes may make important contributions to the aerosol, but are not included here. This organic fractionation framework is an initial step towards a closer linking of ocean biogeochemistry and aerosol chemical composition in Earth system models. Future work should focus on improving constraints on model parameters through new laboratory experiments or through empirical fitting to observed relationships in the real ocean and atmosphere, as well as on atmospheric implications of the variable composition of organic matter in sea spray.

Calcium bridging drives polysaccharide co-adsorption to a proxy sea surface microlayer

2021 ◽  
Author(s):  
Kimberly Anne Carter-Fenk ◽  
Abigal Dommer ◽  
Michelle E. Fiamingo ◽  
Jeongin Kim ◽  
Rommie Amaro ◽  
...  
Keyword(s):  
Organic Carbon ◽  
Mass Fraction ◽  
Co Adsorption ◽  
Ocean Surface ◽  
Sea Surface ◽  
Sea Spray ◽  
Surface Microlayer ◽  
Sea Surface Microlayer ◽  
Sea Spray Aerosol ◽  
Significant Mass

Saccharides comprise a significant mass fraction of organic carbon in sea spray aerosol (SSA), but the mechanisms through which saccharides are transferred from seawater to the ocean surface and eventually...

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