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 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.

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.

scholarly journals Diverse Chemical Mixing States of Aerosol Particles in the Southeastern United States

2018 ◽  
Author(s):  
Amy L. Bondy ◽  
Daniel Bonanno ◽  
Ryan C. Moffet ◽  
Bingbing Wang ◽  
Alexander Laskin ◽  
...  
Keyword(s):  
Chemical Species ◽  
Accumulation Mode ◽  
X Ray ◽  
Internal Mixing ◽  
Scanning Transmission ◽  
Sea Spray Aerosol ◽  
Cloud Activation ◽  
Mixing States ◽  
X Ray Absorption ◽  
Individual Particles

Abstract. Aerosols in the atmosphere are chemically complex with thousands or more chemical species distributed in different proportions across individual particles in an aerosol population. An internal mixing assumption, with species present in the same proportions across all aerosols, is used in many models and calculations of secondary organic aerosol (SOA) formation, cloud activation, and aerosol optical properties. However, many of these effects depend on the distribution of species within individual particles, and important information can be lost when internal mixtures are assumed. Herein, we show that during the Southern Oxidant and Aerosol Study (SOAS) in Centreville, Alabama, at a rural, forested location, that aerosols frequently are not purely internally mixed, even in the accumulation mode (0.2–1.0 µm). A range of aerosol sources and mixing states were obtained using computer controlled scanning electron microscopy with energy dispersive X-ray spectroscopy (CCSEM-EDX) and scanning transmission X-ray microscopy-near-edge X-ray absorption fine structure spectroscopy (STXM-NEXAFS). Particles that were dominated by SOA and inorganic salts were the majority of particles by number fraction from 0.2–5 microns with an average of 78 % SOA in the accumulation mode. However, during certain periods contributions by sea spray aerosol (SSA) and mineral dust were significant to accumulation (22 % SSA and 26 % dust) and coarse mode number concentrations (38 % SSA and 63 % dust). The fraction of particles containing key elements (Na, Mg, K, Ca, and Fe) were determined as a function of size for specific classes of particles. Within internally mixed SOA/sulfate particles

Synchrotron-Based Chemical Nano-Tomography of Microbial Cell-Mineral Aggregates in their Natural, Hydrated State

2014 ◽  
Vol 20 (2) ◽  
pp. 531-536 ◽  
Author(s):  
Gregor Schmid ◽  
Fabian Zeitvogel ◽  
Likai Hao ◽  
Pablo Ingino ◽  
Wolfgang Kuerner ◽  
...  
Keyword(s):  
Chemical Composition ◽  
Direct Evidence ◽  
Three Dimensional ◽  
Chemical Species ◽  
Chemical Processes ◽  
Chemical Mapping ◽  
Bacterial Reduction ◽  
X Ray ◽  
Scanning Transmission ◽  
Projection Images

AbstractChemical nano-tomography of microbial cells in their natural, hydrated state provides direct evidence of metabolic and chemical processes. Cells of the nitrate-reducing Acidovorax sp. strain BoFeN1 were cultured in the presence of ferrous iron. Bacterial reduction of nitrate causes precipitation of Fe(III)-(oxyhydr)oxides in the periplasm and in direct vicinity of the cells. Nanoliter aliquots of cell-suspension were injected into custom-designed sample holders wherein polyimide membranes collapse around the cells by capillary forces. The immobilized, hydrated cells were analyzed by synchrotron-based scanning transmission X-ray microscopy in combination with angle-scan tomography. This approach provides three-dimensional (3D) maps of the chemical species in the sample by employing their intrinsic near-edge X-ray absorption properties. The cells were scanned through the focus of a monochromatic soft X-ray beam at different, chemically specific X-ray energies to acquire projection images of their corresponding X-ray absorbance. Based on these images, chemical composition maps were then calculated. Acquiring projections at different tilt angles allowed for 3D reconstruction of the chemical composition. Our approach allows for 3D chemical mapping of hydrated samples and thus provides direct evidence for the localization of metabolic and chemical processes in situ.

scholarly journals Wind speed dependent size-resolved parameterization for the organic enrichment of sea spray

2011 ◽  
Vol 11 (4) ◽  
pp. 10525-10555 ◽  
Author(s):  
B. Gantt ◽  
N. Meskhidze ◽  
M. C. Facchini ◽  
M. Rinaldi ◽  
D. Ceburnis ◽  
...  
Keyword(s):  
Chemical Composition ◽  
Wind Speed ◽  
Organic Carbon ◽  
Chlorophyll A ◽  
Surface Wind ◽  
Surface Wind Speed ◽  
Organic Enrichment ◽  
Significant Source ◽  
Sea Spray ◽  
Chl A

Abstract. For oceans to become a significant source of primary organic aerosol (POA), sea spray 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 (OMss). 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 OMss. This relationship, combined the published aerosol size dependence of OMss, resulted in a new parameterization for the organic carbon fraction of sea spray. Global marine primary organic emission is investigated here by applying this newly-developed relationship to existing sea spray emission functions, satellite-derived [Chl-a], and modeled 10 meter winds. Analysis of model simulations show 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.

Sea spray aerosol chemical composition: elemental and molecular mimics for laboratory studies of heterogeneous and multiphase reactions

2018 ◽  
Vol 47 (7) ◽  
pp. 2374-2400 ◽  
Author(s):  
Timothy H. Bertram ◽  
Richard E. Cochran ◽  
Vicki H. Grassian ◽  
Elizabeth A. Stone
Keyword(s):  
Chemical Composition ◽  
Aerosol Particle ◽  
Sea Spray ◽  
Laboratory Studies ◽  
Organic Film ◽  
Schematic Representation ◽  
Multiphase Reactions ◽  
Sea Spray Aerosol ◽  
Aerosol Chemical Composition

Schematic representation of the reactive uptake of N2O5to a sea spray aerosol particle containing a thick organic film.

scholarly journals Secondary Marine Aerosol Plays a Dominant Role over Primary Sea Spray Aerosol in Cloud Formation

2020 ◽  
Vol 6 (12) ◽  
pp. 2259-2266
Author(s):  
Kathryn J. Mayer ◽  
Xiaofei Wang ◽  
Mitchell V. Santander ◽  
Brock A. Mitts ◽  
Jonathan S. Sauer ◽  
...  
Keyword(s):  
Dominant Role ◽  
Cloud Formation ◽  
Sea Spray ◽  
Marine Aerosol ◽  
Sea Spray Aerosol

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 A Link between the Ice Nucleation Activity of Sea Spray Aerosol and the Biogeochemistry of Seawater

2020 ◽  
Author(s):  
Martin J. Wolf ◽  
Megan Goodell ◽  
Eric Dong ◽  
Lilian A. Dove ◽  
Cuiqi Zhang ◽  
...  
Keyword(s):  
North Pacific Ocean ◽  
Ice Nucleation ◽  
Cloud Formation ◽  
Subsurface Water ◽  
Sea Spray ◽  
Subsurface Waters ◽  
Sea Spray Aerosol ◽  
Nucleation Activity ◽  
Florida Straits ◽  
Ice Nucleation Activity

Abstract. Emissions of ice nucleating particles from sea spray can impact climate and precipitation by changing cloud formation, precipitation, and albedo. However, the relationship between seawater biogeochemistry and the ice nucleation activity of sea spray aerosols remains unclarified. Here, we demonstrate a link between the biological productivity in seawater and the ice nucleation activity of sea spray aerosol under conditions relevant to cirrus and mixed-phase cloud formation. We show for the first time that aerosol generated from both subsurface and microlayer seawater from the highly productive Eastern Tropical North Pacific Ocean are effective ice nucleating particles in the deposition and immersion freezing modes. Jet droplets aerosolized from the subsurface waters of highly productive regions may therefore be an unrealized source of effective INPs. In contrast, the subsurface water from the less productive Florida Straits produced less effective immersion mode INPs and ineffective depositional mode INPs. These results indicate that the regional biogeochemistry of seawater can strongly affect the ice nucleation activity of sea spray aerosol.

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