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 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 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.

The changing nature of particulate organic carbon and the relation to aerosol liquid water

2020 ◽  
Author(s):  
Annmarie Carlton ◽  
Amy Christiansen ◽  
William Porter ◽  
Madison Flesch
Keyword(s):  
Organic Carbon ◽  
Particulate Organic Carbon ◽  
Liquid Water ◽  
Phase State ◽  
Monitoring Network ◽  
Particle Phase ◽  
Organic Mass ◽  
West Texas ◽  
Isoprene Oxidation ◽  
Mass Concentrations

<p>Particulate organic carbon (OC) mass concentrations demonstrate decreasing trends in many regions across the contiguous US (CONUS). We investigate decadal trends in specific total organic carbon (TOC) volatility fractions OC1, OC2, OC3, and OC4 as defined and reported at 121 locations in the Interagency Monitoring of PROtected Visual Environments (IMPROVE) monitoring network from 2005-2016 for 23 chemical climatology regions across the CONUS. Volatility fraction OC2 drives ubiquitous decadal decreases in TOC, and OC3 mass concentrations increase. The largest changes in OC2 and OC3 occur in the eastern US. In four focus regions (Northeast, Appalachia, West Texas, and Northwest), OC fraction mass concentrations are converted to organic mass (OM) using region-specific OM:OC ratios. GEOS-Chem simulations reproduce and correlate strongly (R<sup>2</sup>>0.7) with OM fraction decadal trends. Decreases in aerosol liquid water (ALW) concentrations are tightly linked to observed change in individual TOC thermal fractions, and aerosol products derived from aqueous-phase isoprene oxidation predicted by GEOS-Chem. These results lend insight to changing chemical regimes with implications for particle phase state, viscosity, and oxidation state.</p>

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 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...

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

2014 ◽  
Vol 14 (5) ◽  
pp. 5375-5443 ◽  
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 semi-labile 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 non-productive 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 include the formation of marine colloidal particles that may be more efficiently swept up by rising particles, 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.

scholarly journals Secondary Sulfate is Internally Mixed with Sea Spray Aerosol and Organic Aerosol in the Winter-Spring Arctic

2017 ◽  
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 ◽  
Atmospheric Processing ◽  
Arctic Aerosol ◽  
Spring Transition ◽  
Sea Spray Aerosol ◽  
Mixing States

Abstract. Few measurements of aerosol chemical composition have been made during the winter-spring transition to constrain Arctic aerosol-cloud-climate feedbacks. Herein, we report the first measurements of individual particle chemical composition near Utqiaġvik (Barrow), Alaska in winter-spring (January and February 2014). Sea spray aerosol (SSA) was observed in all samples, with fresh and aged SSA comprising 99 %, by number, of 2.5–10 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-spring transition. 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-spring Arctic.

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