scholarly journals A Dynamic Link between Ice Nucleating Particles Released in Nascent Sea Spray Aerosol and Oceanic Biological Activity during Two Mesocosm Experiments

2017 ◽  
Vol 74 (1) ◽  
pp. 151-166 ◽  
Author(s):  
Christina S. McCluskey ◽  
Thomas C. J. Hill ◽  
Francesca Malfatti ◽  
Camille M. Sultana ◽  
Christopher Lee ◽  
...  
Keyword(s):  
Biological Activity ◽  
Heterotrophic Bacteria ◽  
Phytoplankton Bloom ◽  
Sea Spray ◽  
Emission Rates ◽  
Phytoplankton Blooms ◽  
Aerosol Composition ◽  
Chl A ◽  
Mesocosm Experiments ◽  
Sea Spray Aerosol

Abstract Emission rates and properties of ice nucleating particles (INPs) are required for proper representation of aerosol–cloud interactions in atmospheric models. Few investigations have quantified marine INP emissions, a potentially important INP source for remote oceanic regions. Previous studies have suggested INPs in sea spray aerosol (SSA) are linked to oceanic biological activity. This proposed link was explored in this study by measuring INP emissions from nascent SSA during phytoplankton blooms during two mesocosm experiments. In a Marine Aerosol Reference Tank (MART) experiment, a phytoplankton bloom was produced with chlorophyll-a (Chl a) concentrations reaching 39 μg L−1, while Chl a concentrations more representative of natural ocean conditions were obtained during the Investigation into Marine Particle Chemistry and Transfer Science (IMPACTS; peak Chl a of 5 μg L−1) campaign, conducted in the University of California, San Diego, wave flume. Dynamic trends in INP emissions occurred for INPs active at temperatures > −30°C. Increases in INPs active between −25° and −15°C lagged the peak in Chl a in both studies, suggesting a consistent population of INPs associated with the collapse of phytoplankton blooms. Trends in INP emissions were also compared to aerosol composition, abundances of microbes, and enzyme activity. In general, increases in INP concentrations corresponded to increases in organic species in SSA and the emissions of heterotrophic bacteria, suggesting that both microbes and biomolecules contribute to marine INP populations. INP trends were not directly correlated with a single biological marker in either study. Direct measurements of INP chemistry are needed to accurately identify particles types contributing to marine INP populations.

scholarly journals Linking variations in sea spray aerosol particle hygroscopicity to composition during two microcosm experiments

2016 ◽  
Author(s):  
Sara D. Forestieri ◽  
Gavin C. Cornwell ◽  
Taylor M. Helgestad ◽  
Kathryn A. Moore ◽  
Christopher Lee ◽  
...  
Keyword(s):  
Light Scattering ◽  
Relative Humidity ◽  
Salt Content ◽  
Sea Salt ◽  
Sea Spray ◽  
Hygroscopic Growth ◽  
Phytoplankton Blooms ◽  
Aerosol Composition ◽  
Sea Spray Aerosol ◽  
Indoor And Outdoor

Abstract. The extent to which water uptake influences the light scattering ability of marine sea spray aerosol (SSA) particles depends critically on SSA chemical composition. The organic fraction of SSA can increase during phytoplankton blooms, decreasing the salt content and therefore the hygroscopicity of the particles. In this study, subsaturated hygroscopic growth factors at 85 % relative humidity (GF(85 %)) of SSA particles were quantified during two induced phytoplankton blooms in marine aerosol reference tanks (MARTs). One MART was illuminated with fluorescent lights and the other was illuminated with sunlight, referred to as the "indoor" and "outdoor" MARTs, respectively. GF(85 %) values for SSA particles were derived from measurements of light scattering and particle size distributions, concurrently with online single particle and bulk aerosol composition measurements. During both microcosm experiments, the observed bulk average GF(85 %) values were depressed substantially relative to pure, inorganic sea salt, by 10 to 19 %, with a one (indoor MART) and six (outdoor MART) day lag between GF(85 %) depression and the peak chlorophyll-a concentrations. The fraction of organiccontaining SSA particles generally increased after the peak of the phytoplankton blooms. The GF(85 %) values were inversely correlated with the fraction of particles containing organic or other biological markers. This indicates these particles were less hygroscopic than the particles identified as predominately sea salt containing and demonstrates a clear relationship between SSA particle composition and the sensitivity of light scattering to variations in relative humidity. The implications of these observations to the direct climate effects of SSA particles are discussed.

scholarly journals Linking variations in sea spray aerosol particle hygroscopicity to composition during two microcosm experiments

2016 ◽  
Vol 16 (14) ◽  
pp. 9003-9018 ◽  
Author(s):  
Sara D. Forestieri ◽  
Gavin C. Cornwell ◽  
Taylor M. Helgestad ◽  
Kathryn A. Moore ◽  
Christopher Lee ◽  
...  
Keyword(s):  
Organic Matter ◽  
Light Scattering ◽  
Time Lag ◽  
Sea Salt ◽  
Sea Spray ◽  
Phytoplankton Blooms ◽  
Chl A ◽  
Volume Fractions ◽  
Sea Spray Aerosol ◽  
Indoor And Outdoor

Abstract. The extent to which water uptake influences the light scattering ability of marine sea spray aerosol (SSA) particles depends critically on SSA chemical composition. The organic fraction of SSA can increase during phytoplankton blooms, decreasing the salt content and therefore the hygroscopicity of the particles. In this study, subsaturated hygroscopic growth factors at 85 % relative humidity (GF(85 %)) of predominately submicron SSA particles were quantified during two induced phytoplankton blooms in marine aerosol reference tanks (MARTs). One MART was illuminated with fluorescent lights and the other was illuminated with sunlight, referred to as the "indoor" and "outdoor" MARTs, respectively. Optically weighted GF(85 %) values for SSA particles were derived from measurements of light scattering and particle size distributions. The mean optically weighted SSA diameters were 530 and 570 nm for the indoor and outdoor MARTs, respectively. The GF(85 %) measurements were made concurrently with online particle composition measurements, including bulk composition (using an Aerodyne high-resolution aerosol mass spectrometer) and single particle (using an aerosol time-of-flight mass spectrometer) measurement, and a variety of water-composition measurements. During both microcosm experiments, the observed optically weighted GF(85 %) values were depressed substantially relative to pure inorganic sea salt by 5 to 15 %. There was also a time lag between GF(85 %) depression and the peak chlorophyll a (Chl a) concentrations by either 1 (indoor MART) or 3-to-6 (outdoor MART) days. The fraction of organic matter in the SSA particles generally increased after the Chl a peaked, also with a time lag, and ranged from about 0.25 to 0.5 by volume. The observed depression in the GF(85 %) values (relative to pure sea salt) is consistent with the large observed volume fractions of non-refractory organic matter (NR-OM) comprising the SSA. The GF(85 %) values exhibited a reasonable negative correlation with the SSA NR-OM volume fractions after the peak of the blooms (i.e., Chl a maxima); i.e., the GF(85 %) values generally decreased when the NR-OM volume fractions increased. The GF(85 %) vs. NR-OM volume fraction relationship was interpreted using the Zdanovskii–Stokes–Robinson (ZSR) mixing rule and used to estimate the GF(85 %) of the organic matter in the nascent SSA. The estimated pure NR-OM GF(85 %) values were 1.16 ± 0.09 and 1.23 ± 0.10 for the indoor and outdoor MARTS, respectively. These measurements demonstrate a clear relationship between SSA particle composition and the sensitivity of light scattering to variations in relative humidity. The implications of these observations to the direct climate effects of SSA particles are discussed.

scholarly journals Sea spray aerosol organic enrichment, water uptake and surface tension effects

2020 ◽  
Vol 20 (13) ◽  
pp. 7955-7977 ◽  
Author(s):  
Luke T. Cravigan ◽  
Marc D. Mallet ◽  
Petri Vaattovaara ◽  
Mike J. Harvey ◽  
Cliff S. Law ◽  
...  
Keyword(s):  
Surface Tension ◽  
Chlorophyll A ◽  
Water Uptake ◽  
Organic Enrichment ◽  
Sea Spray ◽  
Organic Fraction ◽  
Phytoplankton Blooms ◽  
Aerosol Composition ◽  
Sea Spray Aerosol ◽  
Organic Fractions

Abstract. The aerosol-driven radiative effects on marine low-level cloud represent a large uncertainty in climate simulations, in particular over the Southern Ocean, which is also an important region for sea spray aerosol production. Observations of sea spray aerosol organic enrichment and the resulting impact on water uptake over the remote Southern Hemisphere are scarce, and therefore the region is under-represented in existing parameterisations. The Surface Ocean Aerosol Production (SOAP) voyage was a 23 d voyage which sampled three phytoplankton blooms in the highly productive water of the Chatham Rise, east of New Zealand. In this study we examined the enrichment of organics to nascent sea spray aerosol and the modifications to sea spray aerosol water uptake using in situ chamber measurements of seawater samples taken during the SOAP voyage. Primary marine organics contributed up to 23 % of the sea spray mass for particles with diameter less than approximately 1 µm and up to 79 % of the particle volume for 50 nm diameter sea spray. The composition of the submicron organic fraction was consistent throughout the voyage and was largely composed of a polysaccharide-like component, characterised by very low alkane-to-hydroxyl-concentration ratios of approximately 0.1–0.2. The enrichment of organics was compared to the output from the chlorophyll-a-based sea spray aerosol parameterisation suggested by Gantt et al. (2011) and the OCEANFILMS (Organic Compounds from Ecosystems to Aerosols: Natural Films and Interfaces via Langmuir Molecular Surfactants) models. OCEANFILMS improved on the representation of the organic fraction predicted using chlorophyll a, in particular when the co-adsorption of polysaccharides was included; however, the model still under-predicted the proportion of polysaccharides by an average of 33 %. Nascent 50 nm diameter sea spray aerosol hygroscopic growth factors measured at 90 % relative humidity averaged 1.93±0.08 and did not decrease with increasing sea spray aerosol organic fractions. The observed hygroscopicity was greater than expected from the assumption of full solubility, particularly during the most productive phytoplankton bloom (B1), during which organic fractions were greater than approximately 0.4. The water uptake behaviour observed in this study is consistent with that observed for other measurements of phytoplankton blooms and can be partially attributed to the presence of sea salt hydrates, which lowers the sea spray aerosol hygroscopicity when the organic enrichment is low. The inclusion of surface tension effects only marginally improved the modelled hygroscopicity, and a significant discrepancy between the observed and modelled hygroscopicity at high organic volume fractions remained. The findings from the SOAP voyage highlight the influence of biologically sourced organics on sea spray aerosol composition; these data improve the capacity to parameterise sea spray aerosol organic enrichment and water uptake.

scholarly journals Gaseous chemistry and aerosol mechanism developments for version 3.5.1 of the online regional model, WRF-Chem

2014 ◽  
Vol 7 (6) ◽  
pp. 2557-2579 ◽  
Author(s):  
S. Archer-Nicholls ◽  
D. Lowe ◽  
S. Utembe ◽  
J. Allan ◽  
R. A. Zaveri ◽  
...  
Keyword(s):  
Gas Phase ◽  
Chemical Mechanism ◽  
Reduced Form ◽  
Sea Spray ◽  
Wind Fields ◽  
Aerosol Composition ◽  
Aerosol Emission ◽  
Sea Spray Aerosol ◽  
The Impact ◽  
Phase Chemical

Abstract. We have made a number of developments to the Weather, Research and Forecasting model coupled with Chemistry (WRF-Chem), with the aim of improving model prediction of trace atmospheric gas-phase chemical and aerosol composition, and of interactions between air quality and weather. A reduced form of the Common Reactive Intermediates gas-phase chemical mechanism (CRIv2-R5) has been added, using the Kinetic Pre-Processor (KPP) interface, to enable more explicit simulation of VOC degradation. N2O5 heterogeneous chemistry has been added to the existing sectional MOSAIC aerosol module, and coupled to both the CRIv2-R5 and existing CBM-Z gas-phase schemes. Modifications have also been made to the sea-spray aerosol emission representation, allowing the inclusion of primary organic material in sea-spray aerosol. We have worked on the European domain, with a particular focus on making the model suitable for the study of nighttime chemistry and oxidation by the nitrate radical in the UK atmosphere. Driven by appropriate emissions, wind fields and chemical boundary conditions, implementation of the different developments are illustrated, using a modified version of WRF-Chem 3.4.1, in order to demonstrate the impact that these changes have in the Northwest European domain. These developments are publicly available in WRF-Chem from version 3.5.1 onwards.

scholarly journals Phytoplankton blooms weakly influence the cloud forming ability of sea spray aerosol

2016 ◽  
Vol 43 (18) ◽  
pp. 9975-9983 ◽  
Author(s):  
Douglas B. Collins ◽  
Timothy H. Bertram ◽  
Camille M. Sultana ◽  
Christopher Lee ◽  
Jessica L. Axson ◽  
...  
Keyword(s):  
Sea Spray ◽  
Phytoplankton Blooms ◽  
Sea Spray Aerosol

Size-Dependent Changes in Sea Spray Aerosol Composition and Properties with Different Seawater Conditions

2013 ◽  
Vol 47 (11) ◽  
pp. 5603-5612 ◽  
Author(s):  
Andrew P. Ault ◽  
Ryan C. Moffet ◽  
Jonas Baltrusaitis ◽  
Douglas B. Collins ◽  
Matthew J. Ruppel ◽  
...  
Keyword(s):  
Sea Spray ◽  
Aerosol Composition ◽  
Size Dependent ◽  
Sea Spray Aerosol

scholarly journals Wintertime Arctic Sea Spray Aerosol Composition Controlled by Sea Ice Lead Microbiology

2019 ◽  
Vol 5 (11) ◽  
pp. 1760-1767 ◽  
Author(s):  
Rachel M. Kirpes ◽  
Daniel Bonanno ◽  
Nathaniel W. May ◽  
Matthew Fraund ◽  
Anna J. Barget ◽  
...  
Keyword(s):  
Sea Ice ◽  
Sea Spray ◽  
Aerosol Composition ◽  
Arctic Sea ◽  
Sea Spray Aerosol

scholarly journals Factors driving the seasonal and hourly variability of sea-spray aerosol number in the North Atlantic

2019 ◽  
Vol 116 (41) ◽  
pp. 20309-20314 ◽  
Author(s):  
Georges Saliba ◽  
Chia-Li Chen ◽  
Savannah Lewis ◽  
Lynn M. Russell ◽  
Laura-Helena Rivellini ◽  
...  
Keyword(s):  
Wind Speed ◽  
North Atlantic ◽  
Climate Models ◽  
Marine Boundary Layer ◽  
Phytoplankton Bloom ◽  
Cloud Condensation Nuclei ◽  
Sea Spray ◽  
Wind Speeds ◽  
The North ◽  
Sea Spray Aerosol

Four North Atlantic Aerosol and Marine Ecosystems Study (NAAMES) field campaigns from winter 2015 through spring 2018 sampled an extensive set of oceanographic and atmospheric parameters during the annual phytoplankton bloom cycle. This unique dataset provides four seasons of open-ocean observations of wind speed, sea surface temperature (SST), seawater particle attenuation at 660 nm (cp,660, a measure of ocean particulate organic carbon), bacterial production rates, and sea-spray aerosol size distributions and number concentrations (NSSA). The NAAMES measurements show moderate to strong correlations (0.56 < R < 0.70) between NSSA and local wind speeds in the marine boundary layer on hourly timescales, but this relationship weakens in the campaign averages that represent each season, in part because of the reduction in range of wind speed by multiday averaging. NSSA correlates weakly with seawater cp,660 (R = 0.36, P << 0.01), but the correlation with cp,660, is improved (R = 0.51, P < 0.05) for periods of low wind speeds. In addition, NAAMES measurements provide observational dependence of SSA mode diameter (dm) on SST, with dm increasing to larger sizes at higher SST (R = 0.60, P << 0.01) on hourly timescales. These results imply that climate models using bimodal SSA parameterizations to wind speed rather than a single SSA mode that varies with SST may overestimate SSA number concentrations (hence cloud condensation nuclei) by a factor of 4 to 7 and may underestimate SSA scattering (hence direct radiative effects) by a factor of 2 to 5, in addition to overpredicting variability in SSA scattering from wind speed by a factor of 5.

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 Parameterization of oceanic whitecap fraction based on satellite observations

2016 ◽  
Vol 16 (21) ◽  
pp. 13725-13751 ◽  
Author(s):  
Monique F. M. A. Albert ◽  
Magdalena D. Anguelova ◽  
Astrid M. M. Manders ◽  
Martijn Schaap ◽  
Gerrit de Leeuw
Keyword(s):  
Wind Speed ◽  
Regional Scale ◽  
Global Scale ◽  
Sea Spray ◽  
Emission Rates ◽  
Data Set ◽  
Starting Point ◽  
Different Seasons ◽  
Sea Spray Aerosol ◽  
Intrinsic Correlation

Abstract. In this study, the utility of satellite-based whitecap fraction (W) data for the prediction of sea spray aerosol (SSA) emission rates is explored. More specifically, the study aims at evaluating how an account for natural variability of whitecaps in the W parameterization would affect SSA mass flux predictions when using a sea spray source function (SSSF) based on the discrete whitecap method. The starting point is a data set containing W data for 2006 together with matching wind speed U10 and sea surface temperature (SST) T. Whitecap fraction W was estimated from observations of the ocean surface brightness temperature TB by satellite-borne radiometers at two frequencies (10 and 37 GHz). A global-scale assessment of the data set yielded approximately quadratic correlation between W and U10. A new global W(U10) parameterization was developed and used to evaluate an intrinsic correlation between W and U10 that could have been introduced while estimating W from TB. A regional-scale analysis over different seasons indicated significant differences of the coefficients of regional W(U10) relationships. The effect of SST on W is explicitly accounted for in a new W(U10, T) parameterization. The analysis of W values obtained with the new W(U10) and W(U10, T) parameterizations indicates that the influence of secondary factors on W is for the largest part embedded in the exponent of the wind speed dependence. In addition, the W(U10, T) parameterization is able to partially model the spread (or variability) of the satellite-based W data. The satellite-based parameterization W(U10, T) was applied in an SSSF to estimate the global SSA emission rate. The thus obtained SSA production rate for 2006 of 4.4  ×  1012 kg year−1 is within previously reported estimates, however with distinctly different spatial distribution.

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