Spray Aerosol Research Articles

Constraining the Effect of Surfactants on the Hygroscopic Growth of Model Sea Spray Aerosol Particles

The cloud condensation nuclei activation of sea spray aerosol (SSA) is tightly linked to the hygroscopic properties of these particles and is defined by their physical and chemical properties. While hygroscopic sea salt in SSA strongly influences particle water uptake, the marine-derived components that make up the organic fraction of SSA constitute a complex mixture, and their effect on hygroscopic growth is unknown. To constrain the effect of organic compounds and specifically surface-active compounds that adsorb on particle interfaces, particle hygroscopic growth studies were performed on laboratory-generated model sea salt/sugar particles. For sea salt/glucose particles, ionic surfactants facilitated water uptake at low relative humidity (RH), increasing the particle growth factor (GF) by up to 7.61%, and caused a reduction in the deliquescence relative humidity (DRH), while nonionic surfactants had a minimal effect. Replacing glucose with polysaccharide laminarin in sea salt/sugar/surfactant particles caused a reduction in GF at low RHs and minimized the effect of ionic surfactants on the DRH. At RHs above the DRH, the addition of anionic or nonionic surfactants caused a decrease in GF for both sea salt/glucose and sea salt/laminarin particles. The addition of cationic surfactants, however, did not have a dampening effect on water uptake of sea salt/sugar particles and even showed a GF increase of up to 3.7% at 90% RH. An increase in the complexity of the sugar dampens the water uptake for particles containing nonionic surfactants but increases the water uptake for cationic surfactants. The cloud activation potential for 100 nm particles analyzed in this study is higher for ionic surfactants and decreases with an increase in surfactant molecular size when particle interfacial tension is considered. The surfactant effect on the hygroscopic growth and cloud activation potential of the particles containing sea salt/sugar is dependent on the surfactant ionicity and molecular size, the particle size and interfacial tension, and the interactions between inorganic salt and organic species under different RH conditions.

Characterization of adhesivity of organic enriched sea spray aerosols by atomic force microscopy

Aerosol particles can trigger various environmental issues, not only when they are airborne but even after their deposition. For example, highly corrosive sea spray aerosols (SSA) can be deposited on surfaces and cause damage to steel- or concrete-based infrastructure, especially in coastal areas. However, the extent to which the adhesive behavior of SSA is affected by different degrees of organic mixing has not been sufficiently studied. The goal of this study was to evaluate the adhesion forces of both laboratory-generated and ambient SSA with a variety of organic contents on an individual particle basis using atomic force microscopy. Aerosols were also generated using a bulk sea foam sample collected from the coast of Noto Peninsula, Japan to simulate SSA enriched in a complex mixture of marine organics. The adhesion force of the sea foam particles was compared with that of two types of standard monosaccharides (glucose and fucose), artificial inorganic sea salt (ASS), glucose and ASS mixtures at different mass ratios, and ambient sea salt (SS) particles. Pure monosaccharide or its mixtures showed substantially larger adhesion forces than predominantly inorganic particles such as ASS and SS. In addition, it was found that a fraction of sea foam particles showed similarly large adhesion forces, suggesting that organic (e.g., monosaccharides)-enriched SSA can be considerably more adhesive than inorganic salts. Furthermore, a few but surprisingly adhesive particles were also identified among ambient aerosols. Therefore, it is necessary to consider the abundance of organics such as saccharides to correctly evaluate the adhesivity of SSA.

Anthropogenic and Biogenic Contributions to the Organic Composition of Coastal Submicron Sea Spray Aerosol.

The organic composition of coastal sea spray aerosol is important for both atmospheric chemistry and public health but remains poorly characterized. Coastal waters contain an organic material derived from both anthropogenic processes, such as wastewater discharge, and biological processes, including biological blooms. Here, we probe the chemical composition of the organic fraction of sea spray aerosol over the course of the 2019 SeaSCAPE mesocosm experiment, in which a phytoplankton bloom was facilitated in natural coastal water from La Jolla, California. We apply untargeted two-dimensional gas chromatography to characterize submicron nascent sea spray aerosol samples, reporting ∼750 unique organic species traced over a 19 day phytoplankton bloom experiment. Categorization and quantitative compositional analysis reveal three major findings. First, anthropogenic species made up 30% of total submicron nascent sea spray aerosol organic mass under the pre-bloom condition. Second, biological activity drove large changes within the aerosolized carbon pool, decreasing the anthropogenic mass fraction by 89% and increasing the biogenic and biologically transformed fraction by a factor of 5.6. Third, biogenic marine organics are underrepresented in mass spectral databases in comparison to marine organic pollutants, with more than twice as much biogenic aerosol mass attributable to unlisted compounds.

Ice-nucleating agents in sea spray aerosol identified and quantified with a holistic multimodal freezing model.

Sea spray aerosol (SSA) is a widely recognized important source of ice-nucleating particles (INPs) in the atmosphere. However, composition-specific identification, nucleation processes, and ice nucleation rates of SSA-INPs have not been well constrained. Microspectroscopic characterization of ambient and laboratory-generated SSA confirms that water-borne exudates from planktonic microorganisms composed of a mixture of proteinaceous and polysaccharidic compounds act as ice-nucleating agents (INAs). These data and data from previously published mesocosm and wave channel studies are subsequently used to further develop the stochastic freezing model (SFM) producing ice nucleation rate coefficients for SSA-INPs. The SFM simultaneously predicts immersion freezing and deposition and homogeneous ice nucleation by SSA particles under tropospheric conditions. Predicted INP concentrations agree with ambient and laboratory measurements. In addition, this holistic freezing model is independent of the source and exact composition of the SSA particles, making it well suited for implementation in cloud and climate models.

Bubbles spray aerosols: Certitudes and mysteries.

Ocean spray aerosol formed by bubble bursting are at the core of a broad range of atmospheric processes: they are efficient cloud condensation nuclei and carry a variety of chemical, biological, and biomass material from the surface of the ocean to the atmosphere. The origin and composition of these aerosols is sensibly controlled by the detailed fluid mechanics of bubble bursting. This perspective summarizes our present-day knowledge on how bursting bubbles at the surface of a liquid pool contribute to its fragmentation, namely to the formation of droplets stripped from the pool, and associated mechanisms. In particular, we describe bounds and yields for each distinct mechanism, and the way they are sensitive to the bubble production and environmental conditions. We also underline the consequences of each mechanism on some of the many air-sea interactions phenomena identified to date. Attention is specifically payed at delimiting the known from the unknown and the certitudes from the speculations.

Effects of temperature and salinity on bubble-bursting aerosol formation simulated with a bubble-generating chamber

Abstract. A new bubble-generating glass chamber with an extensive set of aerosol production experiments is presented. Compared to the experiments described in the literature since the ground-setting works of Edward C.​​​​​​​ Monahan et al. in 1980s, the current setup is among the medium-sized installations allowing for accurate control of the air discharge, water temperature, and salinity. The size and material of the chamber offer a variety of applications due to its portability, measurement setup adjustability, and sterilization option. The experiments have been conducted in a cylindrical bubbling tank of 10 L volume that was filled by ∼ 30 %–40 % with water of controlled salt content and temperature and covered with a hermetic lid. The chamber was used to study the characteristics of aerosols produced by bursting bubbles under different conditions. In line with previous findings, the sea spray aerosol production was shown to depend linearly on the surface area covered by the bubbles, which in turn is a near-linear function of the air discharge through the water. Observed dependencies of the aerosol size spectra and particle fluxes on water salinity and temperature, being qualitatively comparable with the previous experiments, substantially refined the existing parameterizations. In particular, the bubble size was practically independent from the air discharge through the water body, except in the case of very small flows. Also, the dependence of aerosol spectrum and amount on salinity was much weaker than suggested in some previous experiments. The temperature dependence, to the contrary, was significant and consistent, with a transition in the spectrum shape at ∼ 10 ∘C. Theoretical analysis based on the basic conservation laws supported the main results of the experiments but also highlighted the need for a better understanding of the aerosol production from a cold water surface.

Effects of Atmospheric Aging Processes on Nascent Sea Spray Aerosol Physicochemical Properties.

The effects of atmospheric aging on single-particle nascent sea spray aerosol (nSSA) physicochemical properties, such as morphology, composition, phase state, and water uptake, are important to understanding their impacts on the Earth's climate. The present study investigates these properties by focusing on the aged SSA (size range of 0.1-0.6 μm) and comparing with a similar size range nSSA, both generated at a peak of a phytoplankton bloom during a mesocosm study. The aged SSAs were generated by exposing nSSA to OH radicals with exposures equivalent to 4-5 days of atmospheric aging. Complementary filter-based thermal optical analysis, atomic force microscopy (AFM), and AFM photothermal infrared spectroscopy were utilized. Both nSSA and aged SSA showed an increase in the organic mass fraction with decreasing particle sizes. In addition, aging results in a further increase of the organic mass fraction, which can be attributed to new particle formation and oxidation of volatile organic compounds followed by condensation on pre-existing particles. The results are consistent with single-particle measurements that showed a relative increase in the abundance of aged SSA core-shells with significantly higher organic coating thickness, relative to nSSA. Increased hygroscopicity was observed for aged SSA core-shells, which had more oxygenated organic species. Rounded nSSA and aged SSA had similar hygroscopicity and no apparent changes in the composition. The observed changes in aged SSA physicochemical properties showed a significant size-dependence and particle-to-particle variability. Overall, results showed that the atmospheric aging can significantly influence the nSSA physicochemical properties, thus altering the SSA effects on the climate.

Spatiotemporally Resolved pH Measurement in Aerosol Microdroplets Undergoing Chloride Depletion: An Application of In Situ Raman Microspectrometry.

Acidity is a defining property of atmospheric aerosols that profoundly affects environmental systems, human health, and climate. However, directly measuring the pH of aerosol microdroplets remains a challenge, especially when the microdroplets' composition is nonhomogeneous or dynamically evolving or both. As a result, a pH measurement technique with high spatiotemporal resolution is needed. Here, we report a spatiotemporally resolved pH measurement technique in microdroplets using spontaneous Raman spectroscopy. Our target sample was the microdroplets comprising sodium chloride and oxalic acid─laboratory surrogates of sea spray aerosols and water-soluble organic compounds, respectively. Our measurements show that the chloride depletion from the microdroplets caused a continuous increase in pH by ∼0.5 units in 2 hours. Meanwhile, the surface propensity of chloride anions triggers a stable pH gradient inside a single droplet, with the pH at the droplet surface lower than that at the core by ∼ 0.4 units. The uncertainties arising from the Raman detection limit (±0.08 pH units) and from the nonideal solution conditions (-0.06 pH units) are constrained. Our findings indicate that spontaneous Raman spectroscopy is a simple yet robust technique for precise pH measurement in aerosols with high spatiotemporal resolution.

Opposing comparable large effects of fine aerosols and coarse sea spray on marine warm clouds

Fine aerosols, by acting as cloud condensation nuclei, suppress rainfall and enhance the albedo and coverage of marine warm clouds, thereby partly counteracting the greenhouse-induced warming. While this is relatively well documented, the co-existing opposite effects of giant cloud condensation nuclei from coarse sea spray aerosols are poorly quantified. Here, satellite measurements show that the effects of coarse sea spray aerosols have comparable magnitudes with opposite sign to those of fine aerosols. For fixed cloud liquid water path and coarse sea spray aerosols, increasing fine aerosols decreased rainfall flux and cloud drop effective radius by a factor of 1/4 and 40%, respectively. Conversely, for fixed fine aerosols and cloud liquid water path, added coarse sea spray aerosols enhanced rainfall flux and cloud drop effective radius by a factor of 4 and 35%, respectively. These large and contrasting effects are independent on meteorological conditions. These processes must be fully incorporated into climate models to faithfully represent aerosol effects on clouds, precipitation, and radiative forcing.

Ice-nucleating particles near two major dust source regions

Abstract. Mineral dust and sea spray aerosol represent important sources of ice-nucleating particles (INPs), the minor fraction of aerosol particles able to trigger cloud ice crystal formation and, consequently, influence multiple climate-relevant cloud properties including lifetime, radiative properties and precipitation initiation efficiency. Mineral dust is considered the dominant INP source in many parts of the world due to its ice nucleation efficiency and its sheer abundance, with global emission rates of up to 4700 Tg a−1. However, INPs emitted from the ocean surface in sea spray aerosol frequently dominate INP populations in remote marine environments, including parts of the Southern Ocean where cloud-resolving model simulations have demonstrated that cloud radiative properties are likely strongly controlled by INPs. Here we report INP concentrations measured in aerosol and seawater samples during Air Quality and Climate Change in the Arabian Basin (AQABA), a shipborne campaign that spanned the Red Sea, Gulf of Aden, Arabian Sea, Arabian Gulf and part of the Mediterranean. In aerosol samples collected within a few hundred kilometers of the first and second ranked sources of dust globally, the Sahara and Arabian Peninsula, INP concentrations ranged from 0.2 to 11 L−1 at −20 ∘C with observed ice-active surface site densities (ns) 1–3 orders of magnitude below levels predicted by mineral dust INP parameterizations. Over half of the samples (at least 14 of 26) were collected during dust storms with average dust mass concentrations between 150 and 490 µg m−3 (PM10), as simulated by the Modern-Era Retrospective analysis for Research and Application, version 2 (MERRA-2). The impacts of heat and peroxide treatments indicate that organics dominated the observed ice nucleation (IN) activity at temperatures ≥ −15 ∘C with proteinaceous (heat-labile) INPs frequently observed at high freezing temperatures >−10 ∘C. INP concentrations in seawater samples ranged between 3 and 46 mL−1 at −19 ∘C, demonstrating the relatively low INP source potential of seawater in the region as compared to seawater from multiple other regions reported previously. Overall, our results demonstrate that despite proximity to the Sahara and the Arabian Peninsula and the dominance of mineral dust in the aerosol sampled, existing mineral dust parameterizations alone would not skillfully represent the near-surface ns in the observed temperature regime (−6 to −25 ∘C). Future efforts to develop or improve representations of dust INPs at modest supercooling (≥-15 ∘C) would benefit from a characterization of the specific organic species associated with dust INPs. More generally, an improved understanding of the organic species associated with increased IN activity and their variability across dust source regions would directly inform efforts to determine whether ns-based parameterizations are appropriate for faithful representation of dust INPs in this sensitive temperature regime, whether region-specific parameterizations are required, or whether an alternative to the ns approach is necessary.

Experimental development of a lake spray source function and its model implementation for Great Lakes surface emissions

Abstract. Lake spray aerosols (LSAs) are generated from freshwater breaking waves in a mechanism similar to their saltwater counterparts, sea spray aerosols (SSAs). Unlike the well-established research field pertaining to SSAs, studying LSAs is an emerging research topic due to their potential impacts on regional cloud processes and their association with the aerosolization of freshwater pathogens. A better understanding of these climatic and public health impacts requires the inclusion of LSA emission in atmospheric models, yet a major hurdle to this inclusion is the lack of a lake spray source function (LSSF), namely an LSA emission parameterization. Here, we develop an LSSF based on measurements of foam area and the corresponding LSA emission flux in a marine aerosol reference tank (MART). A sea spray source function (SSSF) is also developed for comparison. The developed LSSF and SSSF are then implemented in the Community Multiscale Air Quality (CMAQ) model to simulate particle emissions from the Great Lakes surface from 10 to 30 November 2016. Measurements in the MART revealed that the average SSA total number concentration was 8 times higher than that of LSA. Over the 0.01–10 µm aerosol diameter size range, the developed LSSF was around 1 order of magnitude lower than the SSSF and around 2 orders of magnitude lower for aerosols with diameters between 1 and 3 µm. Model results revealed that LSA emission flux from the Great Lakes surface can reach ∼105 m−2 s−1 during an episodic event of high wind speeds. These emissions only increased the average total aerosol number concentrations in the region by up to 1.65 %, yet their impact on coarse-mode aerosols was much more significant, with up to a 19-fold increase in some areas. The increase in aerosol loading was mostly near the source region, yet LSA particles were transported up to 1000 km inland. Above the lakes, LSA particles reached the cloud layer, where the total and coarse-mode particle concentrations increased by up to 3 % and 98 %, respectively. Overall, this study helps quantify LSA emission and its impact on regional aerosol loading and the cloud layer.

Probing Individual Particles Generated at the Freshwater-Seawater Interface through Combined Raman, Photothermal Infrared, and X-ray Spectroscopic Characterization.

Sea spray aerosol (SSA) is one of the largest global sources of atmospheric aerosol, but little is known about SSA generated in coastal regions with salinity gradients near estuaries and river outflows. SSA particles are chemically complex with substantial particle-to-particle variability due to changes in water temperature, salinity, and biological activity. In previous studies, the ability to resolve the aerosol composition to the level of individual particles has proven necessary for the accurate parameterization of the direct and indirect aerosol effects; therefore, measurements of individual SSA particles are needed for the characterization of this large source of atmospheric aerosol. An integrated analytical measurement approach is required to probe the chemical composition of individual SSA particles. By combining complementary vibrational microspectroscopic (Raman and optical photothermal infrared, O-PTIR) measurements with elemental information from computer-controlled scanning electron microscopy with energy-dispersive X-ray analysis (CCSEM-EDX), we gained unique insights into the individual particle chemical composition and morphology. Herein, we analyzed particles from four experiments on laboratory-based SSA production using coastal seawater collected in January 2018 from the Gulf of Maine. Individual salt particles were enriched in organics compared to that in natural seawater, both with and without added microalgal filtrate, with greater enrichment observed for smaller particle sizes, as evidenced by higher carbon/sodium ratios. Functional group analysis was carried out using the Raman and infrared spectra collected from individual SSA particles. Additionally, the Raman spectra were compared with a library of Raman spectra consisting of marine-derived organic compounds. Saccharides, followed by fatty acids, were the dominant components of the organic coatings surrounding the salt cores of these particles. This combined Raman, infrared, and X-ray spectroscopic approach will enable further understanding of the factors determining the individual particle composition, which is important for understanding the impacts of SSA produced within estuaries and river outflows, as well as areas of snow and ice melt.

Enrichment of short-chain organic acids transferred to submicron sea spray aerosols

Organic acids, considered to be a substantial component of the marine carbon cycle, can enter the atmosphere through sea spray aerosol (SSA) and further affect the climate. Despite their importance, the distribution and mixing state of organic acids in SSA over the marine boundary layer are poorly understood and therefore need more investigation. Here, we have used ion chromatography (IC) in anion mode to measure short-chain organic acids concentrations in SSA collected throughout a custom-made SSA simulation chamber. The enrichment behavior and morphology of monocarboxylic acids (MAs, C1–8) and dicarboxylic acids (DAs) in submicron SSA were studied in seawater. We found that with MAs addition, the number concentration and mass concentration of SSA particles decreased gradually for C5–8 MAs, whereas they weakly varied with DAs addition due to the fact that carboxyl groups at both ends of DAs increased the surface tension of seawater. Moreover, the target compounds in submicron SSA displayed a surface activity-dependent enrichment behavior, where seawater with stronger surface activity, such as that containing MAs with >5 carbons, was more enriched in SSA in comparison to seawater with weaker surface activity. MAs with chain length <5 carbons were slightly enriched in SSA, whereas the enrichment factor (EF) of C5–8 MAs further increased with increasing chain length. These findings are of utmost importance in further understanding and quantifying the contribution of organic matter to SSA, which is crucial for assessing the atmosphere feedback of the marine carbon cycle. Main finding of the workSurface tension of seawater is the key factor affecting the enrichment of short-chain organic acids in SSA.

Outside the Safe Operating Space of a New Planetary Boundary for Per- and Polyfluoroalkyl Substances (PFAS).

It is hypothesized that environmental contamination by per- and polyfluoroalkyl substances (PFAS) defines a separate planetary boundary and that this boundary has been exceeded. This hypothesis is tested by comparing the levels of four selected perfluoroalkyl acids (PFAAs) (i.e., perfluorooctanesulfonic acid (PFOS), perfluorooctanoic acid (PFOA), perfluorohexanesulfonic acid (PFHxS), and perfluorononanoic acid (PFNA)) in various global environmental media (i.e., rainwater, soils, and surface waters) with recently proposed guideline levels. On the basis of the four PFAAs considered, it is concluded that (1) levels of PFOA and PFOS in rainwater often greatly exceed US Environmental Protection Agency (EPA) Lifetime Drinking Water Health Advisory levels and the sum of the aforementioned four PFAAs (Σ4 PFAS) in rainwater is often above Danish drinking water limit values also based on Σ4 PFAS; (2) levels of PFOS in rainwater are often above Environmental Quality Standard for Inland European Union Surface Water; and (3) atmospheric deposition also leads to global soils being ubiquitously contaminated and to be often above proposed Dutch guideline values. It is, therefore, concluded that the global spread of these four PFAAs in the atmosphere has led to the planetary boundary for chemical pollution being exceeded. Levels of PFAAs in atmospheric deposition are especially poorly reversible because of the high persistence of PFAAs and their ability to continuously cycle in the hydrosphere, including on sea spray aerosols emitted from the oceans. Because of the poor reversibility of environmental exposure to PFAS and their associated effects, it is vitally important that PFAS uses and emissions are rapidly restricted.

Does Sea Spray Aerosol Contribute Significantly to Aerosol Trace Element Loading? A Case Study From the U.S. GEOTRACES Pacific Meridional Transect (GP15)

AbstractAtmospheric deposition represents a major input for micronutrient trace elements (TEs) to the surface ocean and is often quantified indirectly through measurements of aerosol TE concentrations. Sea spray aerosol (SSA) dominates aerosol mass concentration over much of the global ocean, but few studies have assessed its contribution to aerosol TE loading, which could result in overestimates of “new” TE inputs. Low‐mineral aerosol concentrations measured during the U.S. GEOTRACES Pacific Meridional Transect (GP15; 152°W, 56°N to 20°S), along with concurrent towfish sampling of surface seawater, provided an opportunity to investigate this aspect of TE biogeochemical cycling. Central Pacific Ocean surface seawater Al, V, Mn, Fe, Co, Ni, Cu, Zn, and Pb concentrations were combined with aerosol Na data to calculate a “recycled” SSA contribution to aerosol TE loading. Only vanadium was calculated to have a SSA contribution averaging &gt;1% along the transect (mean of 1.5%). We derive scaling factors from previous studies on TE enrichments in the sea surface microlayer and in freshly produced SSA to assess the broader potential for SSA contributions to aerosol TE loading. Maximum applied scaling factors suggest that SSA could contribute significantly to the aerosol loading of some elements (notably V, Cu, and Pb), while for others (e.g., Fe and Al), SSA contributions largely remained &lt;1%. Our study highlights that a lack of focused measurements of TEs in SSA limits our ability to quantify this component of marine aerosol loading and the associated potential for overestimating new TE inputs from atmospheric deposition.

Circum-Antarctic abundance and properties of CCN and INPs

Abstract. Aerosol particles acting as cloud condensation nuclei (CCN) or ice-nucleating particles (INPs) play a major role in the formation and glaciation of clouds. Thereby they exert a strong impact on the radiation budget of the Earth. Data on abundance and properties of both types of particles are sparse, especially for remote areas of the world, such as the Southern Ocean (SO). In this work, we present unique results from ship-borne aerosol-particle-related in situ measurements and filter sampling in the SO region, carried out during the Antarctic Circumnavigation Expedition (ACE) in the austral summer of 2016–2017. An overview of CCN and INP concentrations over the Southern Ocean is provided and, using additional quantities, insights regarding possible CCN and INP sources and origins are presented. CCN number concentrations spanned 2 orders of magnitude, e.g. for a supersaturation of 0.3 % values ranged roughly from 3 to 590 cm−3. CCN showed variable contributions of organic and inorganic material (inter-quartile range of hygroscopicity parameter κ from 0.2 to 0.9). No distinct size dependence of κ was apparent, indicating homogeneous composition across sizes (critical dry diameter on average between 30 and 110 nm). The contribution of sea spray aerosol (SSA) to the CCN number concentration was on average small. Ambient INP number concentrations were measured in the temperature range from −5 to −27 ∘C using an immersion freezing method. Concentrations spanned up to 3 orders of magnitude, e.g. at −16 ∘C from 0.2 to 100 m−3. Elevated values (above 10 m−3 at −16 ∘C) were measured when the research vessel was in the vicinity of land (excluding Antarctica), with lower and more constant concentrations when at sea. This, along with results of backward-trajectory analyses, hints towards terrestrial and/or coastal INP sources being dominant close to ice-free (non-Antarctic) land. In pristine marine areas INPs may originate from both oceanic sources and/or long-range transport. Sampled aerosol particles (PM10) were analysed for sodium and methanesulfonic acid (MSA). Resulting mass concentrations were used as tracers for primary marine and secondary aerosol particles, respectively. Sodium, with an average mass concentration around 2.8 µg m−3, was found to dominate the sampled, identified particle mass. MSA was highly variable over the SO, with mass concentrations up to 0.5 µg m−3 near the sea ice edge. A correlation analysis yielded strong correlations between sodium mass concentration and particle number concentration in the coarse mode, unsurprisingly indicating a significant contribution of SSA to that mode. CCN number concentration was highly correlated with the number concentration of Aitken and accumulation mode particles. This, together with a lack of correlation between sodium mass and Aitken and accumulation mode number concentrations, underlines the important contribution of non-SSA, probably secondarily formed particles, to the CCN population. INP number concentrations did not significantly correlate with any other measured aerosol physico-chemical parameter.

Influence of surfactant concentration on drop production by bubble bursting

Bubble bursting at the surface of the sea water produce drops and is the main source of sea spay aerosol. The mechanisms underlying the drops production from a single bubble bursting event have been intensively studied and the influence of the bubble size and liquid parameters (density, viscosity and surface tension) has been unified. However, despite the diversity of the surfactant molecules present in the oceans, their influence has been overlooked. In this paper we experimentally explore the influence of the surfactant concentration (Sodium Dodecyl Surfate - SDS) in a water solution on a single bubble collapse and subsequent drop production. We show that these surfactant molecules have an astonishing effect. In particular, we quantitatively show that they modify the bubble collapse, they induce less, smaller and faster drops and they can even completely prevent the drop production for a particular concentration. These results are presented in the existing dimensionless framework and they allow us to affirme that these effects are mainly a consequence of the surface tension gradients (Marangoni stresses) more than just the surface tension lowering. Finally, this study shows that the role of water contamination by surface-active agents is important and needs to be understood to improve the prediction of the sea spray aerosol.

Retrieval of the sea spray aerosol mode from submicron particle size distributions and supermicron scattering during LASIC

Abstract. Improved quantification of sea spray aerosol concentration and size is important for determining aerosol effects on clouds and the climate, though attempts to accurately capture the size distribution of the sea spray mode remain limited by the availability of supermicron size distributions. In this work, we introduce a new approach to retrieving lognormal mode fit parameters for a sea spray aerosol mode by combining submicron size distributions with supermicron scattering measurements using a Mie inversion. Submicron size distributions were measured by an ultra-high-sensitivity aerosol spectrometer (UHSAS), and supermicron scattering was taken as the difference between &lt;10 µm and &lt;1 µm three-wavelength integrating nephelometer measurements (NEPH). This UHSAS-NEPH method was applied during background marine periods of the Department of Energy Atmospheric Radiation Measurement Layered Atlantic Smoke Interactions with Clouds (LASIC) campaign on Ascension Island (November 2016–May 2017), when the contribution of sea spray aerosol was expected to represent a large fraction of the aerosol mass and total scattering. Lognormal sea spray modal parameters were retrieved from comparisons between nephelometer measurements and a lookup table of Mie theory-simulated scattering coefficients for low-error solutions that minimized the 0.4–1 µm residual in the UHSAS size distribution. We evaluated the UHSAS-NEPH method with a set of clean marine measurements in the North Atlantic that included supermicron size and chemical measurements, showing that measured supermicron size distributions are needed to constrain the sea spray number concentration but that mass concentration was reasonably characterized using supermicron scattering. For LASIC, the UHSAS-NEPH method retrieved sea spray mode properties for approximately 88 % of the background marine times when the scattering variability and total particle concentration were low (&lt;± 5 Mm−1 and &lt;400 cm−3, respectively), with mass mean diameter ranging from 0.6 to 1.9 µm (1.47 ± 0.17 µm), modal width ranging from 1.1 to 3.97 (2.4±0.3), and mass concentration ranging from 0.18 to 23.0 µg m−3 (8.37. ± 4.1 µg m−3). The measured nephelometer scattering at three wavelengths was found to constrain the mode width marginally at the largest particle sizes in the absence of additional size and chemical measurements for defining parameters for the Mie solutions. Comparing UHSAS-NEPH retrievals to those of a fitting algorithm applied only to the submicron UHSAS number size distribution showed that correlations between retrieved mass concentration and the available mass-based sea spray tracers (coarse scattering, wind speed, and chloride) are low when supermicron measurements are not considered. This work demonstrates the added value of supermicron scattering measurements for retrieving reasonable sea spray mass concentrations, providing the best-available observationally constrained estimate of the sea spray mode properties when supermicron size distribution measurements are not available.

Chemical Composition of an Ultrafine Sea Spray Aerosol during the Sea Spray Chemistry and Particle Evolution Experiment

Chemical Composition of an Ultrafine Sea Spray Aerosol during the Sea Spray Chemistry and Particle Evolution Experiment

Wound healing activity of topical herbal aerosol sprays on diabetic and Varicose Ulcers: A randomized, controlled, open labelled, multi-centric clinical trial

BackgroundPanchavalkala Kwatha and Jatyadi Taila are recommended for cleaning and healing of non-healing ulcers such as Diabetic Foot Ulcer (DFU) and Varicose Ulcers (VU). ObjectivesInnovative topical aerosol sprays viz. Panchavalkala Kwatha Aerosol Spray (PKS) and Jatyadi Taila (Healz) Aerosol Spray (JTS) were evaluated for healing in DFU & VU against conventional treatment. Materials & methodsAfter obtaining approval from Ethics Commitees & informed consent, 53 patients were randomized in two study groups. In one group, ulcer cleaning was done with PKS and then JTS was used for dressing while in other group, cleaning was done with Hydrogen peroxide and/or Hypochlorite followed by dressing with 10% Povidone iodine. Ulcer examination was done from baseline to every 7th day by Bates Jensen ulcer assessment tool, digital photographs and photographic ulcer assessment tool. Comparison of categorical variables was done using t-test. ResultsThe dual action of PKS and JTS exhibited potentially comparable effect to the conventional treatment. ConclusionPKS and JTS were found to be effective, comfortable, hygenic and acceptable in management of chronic ulcers.