Measurements of ocean derived aerosol off the coast of California

Bates, T. S.; Quinn, Patricia K.; Frossard, A. A.; Russell, Lynn M.; Hakala, J.; Petäj̈ä, Tuukka; Kulmala, Markku; Covert, David S.; Cappa, C. D.; Li, S. M.; Hayden, K. L.; Nuaaman, I.; McLaren, R.; Massoli, P.; Canagaratna, Manjula R.; Onasch, T. B.; Sueper, D.; Worsnop, Douglas R.; Keene, W. C.

doi:10.1029/2012jd017588

Cited by 117 publications

(170 citation statements)

References 72 publications

(112 reference statements)

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“…After all dehydration steps were completed, X-ray fluorescence (XRF; Chester LabNet, Tigard, OR) was used to quantify the masses of elements Na, Mg, S, Cl, K, Ca, V, Fe, Br, and Sr. 17 Ambient submicrometer particles were also collected on additional filters using two-stage multijet cascade impactors 18 and analyzed with ion chromatography (IC) to quantify inorganic ions, including Na and Cl. 19,20 1. Laboratory-Generated Reference Standards of Seawater Components.…”

Section: ■ Methodsmentioning

confidence: 99%

Removal of Sea Salt Hydrate Water from Seawater-Derived Samples by Dehydration

Frossard

Russell

2012

Environ. Sci. Technol.

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Aerosol particles produced from bubble bursting of natural seawater contain both sea salts and organic components. Depending on the temperature, pressure, and speed of drying, the salt components can form hydrates that bind water, slowing evaporation of the water, particularly if large particles or thick layers of salts undergo drying that is nonuniform and incomplete. The water bound in these salt hydrates interferes with measuring organic hydroxyl and amine functional groups by Fourier transform infrared (FTIR) spectroscopy because it absorbs at the same infrared wavelengths. Here, a method for separating the hydrate water in sea salt hydrates using freezing and then heating in warm, dry air (70°C) is evaluated and compared to other methods, including spectral subtraction. Laboratory-generated sea salt analogs show an efficient removal of 89% of the hydrate water absorption peak height by 24 h of heating at atmospheric pressure. The heating method was also applied to bubbled submicrometer (Sea Sweep), generated bulk (Bubbler), and atomized seawater samples, with efficient removal of 5, 22, and 39 μg of hydrate water from samples of initial masses of 11, 30, 58 μg, respectively. The strong spectral similarity between the difference of the initial and dehydrated spectra and the laboratory-generated sea salt hydrate spectrum provided verification of the removal of hydrate water. In contrast, samples of submicrometer atmospheric particles from marine air masses did not have detectable signatures of sea salt hydrate absorbance, likely because their smaller particles and lower filter loadings provided higher surface area to volume ratios and allowed faster and more complete drying. ■ INTRODUCTIONSeawater and freshly emitted sea spray particles are 97% water, by mass, but they also contain trace amounts of important organic components. A macroscopic sample of seawater dried to 0% RH can leave up to 15% of the mass of dry sea salt as bound water molecules in hydrates, 1 depending on the morphology of the salt mixture and the method of drying. The rationale for this study was to develop a method for characterizing the organic components of particles produced by seawater bubble bursting (and by other sources such as dust that retain substantial amounts of water bound as hydrates). FTIR spectroscopy has been shown effective for measuring the organic components of salt and dust-containing refractory particles, but the presence of hydrate water interferes with the measurement of organic hydroxyl groups.Evaporated seawater can include halite (NaCl), kieserite (MgSO 4 ·1H 2 O), carnallite (KMgCl 3 ·6H 2 O), anhydrite (CaSO 4 ), and bischofite (MgCl 2 ·6H 2 O). 2 The most abundant salt formed from standard seawater evaporation is NaCl (∼90%) followed by MgCl 2 and MgSO 4 (∼3−4% each) and KMgCl 3 and CaSO 4 (∼2% each). 2 Previous studies have shown absorbance in the infrared (IR) region of hydrate bound and liquid water in salt water mixtures using Fourier transform infrared (FTIR) spectroscopy at differing RH values...

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Section: ■ Methodsmentioning

confidence: 99%

Removal of Sea Salt Hydrate Water from Seawater-Derived Samples by Dehydration

Frossard

Russell

2012

Environ. Sci. Technol.

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“…Temporal profiles for ATOFMS sea salt particle numbers, OPS number concentrations, PILS-IC sea salt aerosol (SSA, calculated using SSA = [Cl − ] + [Na + ] × 1.47; Bates et al, 2012) and ATOFMS fresh sea salt mass concentrations are shown in Fig. 9.…”

Section: Sea Saltmentioning

confidence: 99%

Sources and mixing state of summertime background aerosol in the north-western Mediterranean basin

et al. 2017

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Abstract. An aerosol time-of-flight mass spectrometer (ATOFMS) was employed to provide real-time single particle mixing state and thereby source information for aerosols impacting the western Mediterranean basin during the ChArMEx-ADRIMED and SAF-MED campaigns in summer 2013. The ATOFMS measurements were made at a ground-based remote site on the northern tip of Corsica.Twenty-seven distinct ATOFMS particle classes were identified and subsequently grouped into eight general categories: EC-rich (elemental carbon), K-rich, Na-rich, amines, OC-rich (organic carbon), V-rich, Fe-rich and Carich particles. Mass concentrations were reconstructed for the ATOFMS particle classes and found to be in good agreement with other co-located quantitative measurements (PM 1 , black carbon (BC), organic carbon, sulfate mass and ammonium mass). Total ATOFMS reconstructed mass (PM 2.5 ) accounted for 70-90 % of measured PM 10 mass and was comprised of regionally transported fossil fuel (EC-rich) and biomass burning (K-rich) particles. The accumulation of these transported particles was favoured by repeated and extended periods of air mass stagnation over the western Mediterranean during the sampling campaigns. The single particle mass spectra proved to be valuable source markers, allowing the identification of fossil fuel and biomass burning combustion sources, and was therefore highly complementary to quantitative measurements made by Particle into Liquid Sampler ion chromatography (PILS-IC) and an aerosol chemical speciation monitor (ACSM), which have demonstrated that PM 1 and PM 10 were comprised predominantly of sulfate, ammonium and OC. Good temporal agreement was observed between ATOFMS EC-rich and K-rich particle mass concentrations and combined mass concentrations of BC, sulfate, ammonium and low volatility oxygenated organic aerosol (LV-OOA). This combined information suggests that combustion of fossil fuels and biomass produced primary EC-and OC-containing particles, which then accumulated ammonium, sulfate and alkylamines during regional transport.Three other sources were also identified: local biomass burning, marine and shipping. Local combustion particlesPublished by Copernicus Publications on behalf of the European Geosciences Union. (emitted in Corsica) contributed little to PM 2.5 particle number and mass concentrations but were easily distinguished from regional combustion particles. Marine emissions comprised fresh and aged sea salt: the former was detected mostly during a 5-day event during which it accounted for 50-80 % of sea salt aerosol mass, while the latter was detected throughout the sampling period. Dust was not efficiently detected by the ATOFMS, and support measurements showed that it was mainly in the PM 2.5-10 fraction. Shipping particles, identified using markers for heavy fuel oil combustion, were associated with regional emissions and represented only a small fraction of PM 2.5 particle number and mass concentration at the site.

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“…Modelling studies have included marine aerosol organic fraction parameterizations to estimate aerosol emission fluxes (Albert et al, 2012;Vignati et al, 2010) and cloud condensation nuclei (CCN) concentrations (Westervelt et al, 2012). Other studies have observed correlations between the aerosol organic fraction and heterotrophic bacteria abundance Schwier et al, 2015), transparent exopolymer particle (TEP) abundance or dimethyl-sulfide concentrations (Bates et al, 2012). However, Ceburnis et al (2016) and Rinaldi et al (2013) observed an anti-correlation between aerosol organic fraction and wind speed at 10 m above the sea surface at Mace Head, Ireland, that could indicate a significant contribution of secondary organic sources to the ambient aerosol organic content.…”

Section: Introductionmentioning

confidence: 99%

Primary marine aerosol physical flux and chemical composition during a nutrient enrichment experiment in mesocosms in the Mediterranean Sea

et al. 2017

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Abstract. While primary marine aerosol (PMA) is an important part of global aerosol total emissions, its chemical composition and physical flux as a function of the biogeochemical properties of the seawater still remain highly uncharacterized due to the multiplicity of physical, chemical and biological parameters that are involved in the emission process. Here, two nutrient-enriched mesocosms and one control mesocosm, both filled with Mediterranean seawater, were studied over a 3-week period. PMA generated from the mesocosm waters were characterized in term of chemical composition, size distribution and size-segregated cloud condensation nuclei (CCN), as a function of the seawater chlorophyll a (Chl a) concentration, pigment composition, virus and bacteria abundances. The aerosol number size distribution flux was primarily affected by the seawater temperature and did not vary significantly from one mesocosm to the other. The aerosol number size distribution flux was primarily affected by the seawater temperature and did not vary significantly from one mesocosm to the other. Particle number and CCN aerosol fluxes increase by a factor of 2 when the temperature increases from 22 to 32 • C, for all particle submicron sizes. This effect, rarely observed in previous studies, could be specific to oligotrophic waters and/or to this temperature range. In all mesocosms (enriched and control mesocosms), we detected an enrichment of calcium (+500 %) and a deficit in chloride (−36 %) in the submicron PMA mass compared to the literature inorganic composition of the seawater. There are indications that the chloride deficit and calcium enrichment are linked to biological processes, as they are found to be stronger in the enriched mesocosms. This implies a non-linear transfer function between the seawater composition and PMA composition, with comPublished by Copernicus Publications on behalf of the European Geosciences Union. plex processes taking place at the interface during the bubble bursting. We found that the artificial phytoplankton bloom did not affect the CCN activation diameter (D p,50,average = 59.85 ± 3.52 nm and D p,50,average = 93.42 ± 5.14 nm for supersaturations of 0.30 and 0.15 % respectively) or the organic fraction of the submicron PMA (average organic to total mass = 0.31 ± 0.07) compared to the control mesocosm. Contrary to previous observations in natural bloom mesocosm experiments, the correlation between the particle organic fraction and the seawater Chl a was poor, indicating that Chl a is likely not a straightforward proxy for predicting, on a daily scale, PMA organic fraction in models for all types of sea and ocean waters. Instead, the organic fraction of the Aitken mode particles were more significantly linked to heterotrophic flagellates, viruses and dissolved organic carbon (DOC). We stress that different conclusions may be obtained in natural (non-enriched) or non-oligotrophic systems.

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Measurements of ocean derived aerosol off the coast of California

Cited by 117 publications

References 72 publications

Removal of Sea Salt Hydrate Water from Seawater-Derived Samples by Dehydration

Removal of Sea Salt Hydrate Water from Seawater-Derived Samples by Dehydration

Sources and mixing state of summertime background aerosol in the north-western Mediterranean basin

Primary marine aerosol physical flux and chemical composition during a nutrient enrichment experiment in mesocosms in the Mediterranean Sea

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