Sea Salt Aerosol Research Articles

Direct photodegradation of internally mixed sodium chloride and malonic acid single aerosols: Impact of the photoproducts on the hygroscopic properties of the particles

Sea-salt aerosols (SSA) are one of the key natural aerosols in our atmosphere, consisting predominantly of sodium chloride (NaCl). Throughout their atmospheric transport, these aerosols undergo complex internal mixing, giving rise to a rich variety of inorganic and organic species, including dicarboxylic acids. This study investigates firstly the composition and deliquescence properties of coarse particles containing pure malonic acid (MA2, CH2(COOH)2) and internally mixed NaCl and MA2, by means of an acoustic levitation system coupled with a Raman microspectrometer. Secondly, we report here the first experimental observation and characterization of the products arising from photochemical reactions under UV–Visible irradiation (338 ≤ λ ≤ 414 nm) in the absence of an oxidant under acoustic levitation conditions in MA2 and NaCl/MA2 aerosols. Furthermore, the impact of photodegradation on the hygroscopic properties of these particles is examined. We confirmed the irreversible formation of monosodium malonate (NaMA, HOOCCH2COONa), which coexists with NaCl or MA2 on non-irradiated particles. We also demonstrated the formation of oxalic acid (OA2, HOOC–COOH) within irradiated MA2 droplets and the appearance of glyoxylic acid (GlyA, HCOCOOH) in NaCl containing droplets. The photolysis process exerts a marked effect on the hygroscopic properties of the particles, resulting in a shift in deliquescence transitions toward higher relative humidity (RH) values. This study contributes to the understanding of the intricate physicochemical processes involved in SSA during their atmospheric transport. Likewise, this work sheds light on the impacts of these types of aerosols on cloud formation and climate change.

Roles of tropical cyclones with varying intensities in the re-distribution of aerosols

The study analyzes three tropical cyclones (TC) with varying intensities, namely BOB02, a deep depression in the Bay of Bengal; Tauktae, an extremely severe cyclone in the Arabian Sea (AS); and Amphan, a supercyclone in the Bay of Bengal, which developed on October 11, 2020, May 13, 2021, and May 16, 2020, respectively. The analysis focuses on studying the re-distribution of the aerosols over the Indian region using these distinct datasets: Modern-Era Retrospective Analysis for Research and Application, version 2 (MERRA2), Integrated Multi-Satellite Retrievals for GPM (IMERG), and Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO). Throughout the cyclonic period, which includes the period from the inception of the low-pressure area to its dissipation as well as the pre-cyclonic and post-cyclonic periods (one week prior to and after the cyclonic period, respectively), various parameters related to aerosols and background meteorological conditions were collected. The primary parameter of interest was the aerosol optical depth (AOD). The analysis revealed significant variations in meteorological parameters such as wind speed, temperature, relative humidity, and rainfall along the cyclone track during both the cyclonic and post-cyclonic conditions compared to the pre-cyclonic conditions of these TCs. The AOD surrounding the cyclone track decreases during cyclonic and post-cyclonic conditions compared to pre-cyclonic conditions. This is due to the scavenging of both anthropogenic and natural (dust) aerosols. Conversely, AOD increases along the cyclone track, mainly due to an increase in natural (sea salt) aerosols. During pre-cyclonic conditions, both natural (dust) and anthropogenic (black carbon, organic carbon, and sulfate) aerosols contribute significantly to the total AOD, whereas during pre-cyclonic conditions, the main contributors are natural (sea-salt) aerosols. The coarse-mode particles are more dominant during cyclonic and post-cyclonic conditions than pre-cyclonic ones. Furthermore, our observations indicate that the atmospheric boundary layer (ABL) height increases by ∼0.1–0.6 km along the cyclone track during cyclonic conditions compared to pre-cyclonic conditions. While AOD from the free troposphere (FT) contributes more to the total AOD, contributions from ABL increase, while those from the FT decrease during cyclonic and post-cyclonic conditions.

Seasonal variation of mercury in cloud water at a mountaintop in subtropical Hong Kong: Influences of transboundary transport and sea-salt aerosol

Understanding the distribution and controlling factors of mercury (Hg) speciation in cloud water is crucial for predicting the fate of atmospheric Hg and assessing the environmental impacts of Hg in cloud water. In this study, we collected 85 cloud water samples during autumn and spring at a mountaintop (957 m a.s.l.) in Hong Kong, China. The concentrations of total Hg (THg) in cloud water varied from 3.6 to 225.3 ng L−1, with volume-weighted mean values of 32.1 ng L−1 in autumn and 24.4 ng L−1 in spring. Due to the strong acidic condition of the cloud water, dissolved Hg (DHg) contributed to two-thirds of THg, with Hg complexes by dissolved organic matter (DOM) and chloride being the predominant species of DHg according to chemical equilibrium modeling simulations. Moreover, the levels of Hg-DOM were significantly higher in autumn cloud water compared to spring, and the latter contained more Hg(II)-halide complexes. These differences could be attributed to the different air mass pathways and their emission sources. By combining backward trajectories and Positive Matrix Factorization (PMF) models, we found that air masses originating from the inland Pearl River Delta region, which were only present in autumn cloud water and strongly influenced by stationary coal combustion, were responsible for the highest concentrations of THg, DHg, particulate Hg (PHg) and Hg-DOM. Additionally, air masses originating from regions in China-Indochina Peninsula were only found in spring samples and were significantly influenced by stationary coal combustion, industrial and biogenic sources, contributing to elevated proportions of methylmercury (MeHg) and PHg. In contrast, marine air masses mainly from the western Pacific Ocean contributed to high levels of Hg(II)-halide complexes, especially in spring cloud water. The dissolution and conversion of Hg from sea salt aerosols played a significant role in the enhanced DHg levels observed during cloud processing.

Fine scale simulation of sea salt aerosol under strong wind: WRF sensitivity test on PBL schemes and LES under Typhoon Hagibis

Identifying which factors among the planetary boundary layer (PBL) scheme, grid resolution, and source or sink terms dominantly influence the sea salt aerosol (SSA) spatial distribution is necessary. The dependence of SSA transport on PBL processes was investigated using a numerical weather prediction (NWP) model with a grid scale of ∼143 m. Size-segregated SSA transport during Typhoon Hagibis, which made landfall in Japan in 2019, was simulated using the Weather Research and Forecasting (WRF) model. The PBL schemes of Yonsei University (YSU), scale-aware YSU (Shin and Hong, 2015's scheme, SH) and Mellor-Yamada Nakanishi-Niino (MYNN), and large-eddy simulation (LES) subjected to turbulence transition enhancement via a cell perturbation method were tested to evaluate the reproducibility of observed values of wind speed, surface pressure, relative humidity, and temperature at meteorology masts. The results showed that wind speed was most influenced by the selection of the PBL scheme and LES. The distance from the coastline, as determined by the wind direction during the most intense typhoon stage, was correlated with a decrease in the time averaged SSA concentration when the storm moved inland. Despite the simulated SSA emission scheme's high sensitivity to wind speed (nearly 3rd power), the near-surface average concentration was less sensitive to the PBL schemes and LES selection than wind speed. However, the maximum arrival of the SSA differed by ∼20 % during the most vigorous stage of the typhoon. Budget analysis of the SSA transport equation highlighted that the advection term and gravity settling were most dependent on the PBL schemes and LES. The impacts of both factors on SSA transport were not limited to near-surface tendencies but were in a broader range over the atmosphere, up to 1–2 km. These results indicated that the vertical structure of the SSA field over the boundary layer depended on the PBL schemes and LES, thereby modulating the inland arrival of the SSA.

Mechanisms controlling giant sea salt aerosol size distributions along a tropical orographic coastline

Abstract. Sea salt aerosol (SSA) is a naturally occurring phenomenon that arises from the breaking of waves and consequent bubble bursting on the ocean's surface. The resulting particles exhibit a bimodal distribution spanning orders of magnitude in size that introduces significant uncertainties when estimating the total annual mass of SSA on a global scale. Although estimates of mass and volume are significantly influenced by the presence of giant particles (dry radius >1 µm), effectively observing and quantifying these particles proves to be challenging. Additionally, uncertainties persist regarding the contribution of SSA production along coastlines, but preliminary studies suggest that coastal interactions may increase SSA particle concentrations by orders of magnitude. Moreover, our knowledge regarding the vertical distribution of SSA particles in the marine boundary layer remains limited, resulting in significant gaps in understanding the vertical mixing of giant aerosol particles and specific environmental conditions facilitating their dispersion. By addressing these uncertainties, particularly in regions where SSA particles constitute a substantial percentage of total aerosol loading, we can enhance our comprehension of the complex relationships between the air, sea, aerosols, and clouds. A case study conducted on the Hawaiian island of O`ahu offers insight into the influence of coastlines and orography on the production and vertical distribution of giant SSA size distributions. Along the coastline, the frequency of breaking waves is accelerated, serving as an additional source of SSA production. Furthermore, the steep island orography generates strong and consistent uplift under onshore trade wind conditions, facilitating vertical mixing of SSA particles along windward coastlines. To investigate this phenomenon, in situ measurements of SSA size distributions for particles with dry radii (rd) ≥ 2.8 µm were conducted for various altitudes, ranging from approximately 80 to 650 m altitude along the windward coastline and from 80 to 250 m altitude aboard a ship offshore. Comparing size distributions onshore and offshore confirmed significantly higher concentrations along the coastline, with 2.7–5.4 times greater concentrations than background open-ocean concentrations for supermicron particles. These size distributions were then analyzed in relation to environmental variables influencing SSA production and atmospheric dynamics. It was found that significant wave height exhibited the strongest correlation with changes in SSA size distributions. Additionally, simulated sea salt particle trajectories provided valuable insight into how production distance from the coastline impacts the horizontal and vertical advection of SSA particles of different sizes under varying trade wind speeds. Notably, smaller particles demonstrated reduced dependence on local wind speeds and production distance from the coastline, experiencing minimal dry deposition and high average maximum altitudes relative to larger particles. This research not only highlights the role of coastlines in enhancing the presence and vertical mixing potential of giant SSA particles, but also emphasizes how important it is to consider the influence of local factors on aerosol observations at different altitudes.

Understanding the origins of and influences on precipitation major ion chemistry on the Island of O'ahu, Hawai'i.

Precipitation is the primary groundwater source for the Island of O'ahu, Hawai'i, USA, and is an important source of terrestrial nutrients. Since Pacific Islands are particularly vulnerable to the impacts of climate change, they are important venues for studying the controls on and fluctuations in precipitation chemistry. Spatial variations in some of the dissolved rainfall ions can also be of value as natural geochemical tracers in examining surface and groundwater flow. This study collected and chemically analyzed bulk precipitation from 20 sites across the Island of O'ahu approximately quarterly between April 2018 and August 2021. The new precipitation chemistry data were integrated with previously published precipitation data to characterize major ion composition and examine the atmospheric processes controlling inorganic ion deposition. Linear regression and multivariate analysis were used to quantify the relationships among major ions and to assess the impacts of various environmental and meteorological factors on precipitation chemistry. Ordinary kriging and inverse distance weighted interpolations were conducted to help visualize spatial variations in major ion deposition. The results clearly indicate that ocean sea spray is the primary driver of precipitation inorganic chemistry, with marine sea salt aerosols accounting for more than 90% of the measured ion load. However, they also show that various weather patterns and nutrient sources impact inorganic deposition. Most notably, upper atmospheric transport of Asian continental dust during Hawaiian wet seasons, Ca2+ from local sedimentary deposits, and anthropogenic K+ from agricultural activity appear to be substantial non-marine deposition sources. This study synthesizes data from multiple sources into the most spatially and topographically diverse precipitation collector network on O'ahu to date. The findings from this effort help establish a baseline for assessing future fluctuations in inorganic ion deposition and lay important groundwork for examining connections between precipitation and groundwater chemistry within the study area.

Low contributions of dimethyl sulfide (DMS) chemistry to atmospheric aerosols over the high Arctic Ocean

The Arctic Ocean is continuously warming, resulting in sea ice retreat, which significantly impacts the marine biogenic sulfur cycle. The formation of aerosols from DMS oxidation and their climatic effects in polar regions are of great concern. However, the impact of DMS chemistry on atmospheric aerosols in the high Arctic Ocean (AO) is still unclear due to the limitation of field observations and datasets. Gaseous methanesulfonic acid (MSA) and aerosol chemical species (MSA, SO42− and DMA, etc.) were determined simultaneously with a high time resolution (1 h) in the AO and Pacific Ocean (PO) to reveal the DMS chemistry in these regions. The particulate MSA concentration indicated significant spatial variation with a decreasing tendency from the low latitude oceans to high AO. Extremely low particulate MSA concentrations were observed in the high AO, with an average of only 7.42 ± 6.6 ng·m−3. In contrast, highest particulate MSA concentrations, with an average of 168.6 ± 167.6 ng·m−3 were observed in the mid-latitude regions (45°–60°N) in July. Sea salt aerosols were the most dominant source in the high Arctic Ocean, accounting for 88.78% of the total suspended particle mass, which was much larger than the values in the other regions. Low DMS chemistry was determined based on the low DMS emissions in the high latitude (HL, 75°–85°N) region. These results highlight the contribution of DMS chemistry to atmospheric aerosols and extend the knowledge of how biogenic aerosols impact the regional atmosphere in the high AO.

Comparison of the Performance of the GRASP and MERRA2 Models in Reproducing Tropospheric Aerosol Layers

Two approaches, based on Generalized Retrieval of Aerosol and Surface Properties (GRASP) and Modern-Era Retrospective Analysis for Research and Applications version 2 (MERRA-2) models, are investigated for reproducing aerosol layers in the troposphere. The GRASP algorithm is supplied with synergistic LIDAR and sunphotometer measurements to obtain aerosol extinction profiles. MERRA-2 is an atmospheric reanalysis coupling model that includes an external mixture of sea salt, dust, organic carbon, black carbon, and sulfate aerosols. A data set from Racibórz observatory, obtained with LIDAR and a sunphotometer in the 2017–2020 period, is analysed with GRASP along with the closest grid point data given by MERRA-2. The models demonstrate satisfactory agreement, yet some discrepancies were observed, indicating the presence of biases. For vertically integrated profiles, the correlation coefficient (R) between aerosol optical thickness was calculated to be 0.84, indicating a strong linear relationship. The Pearson correlation coefficient calculated between profiles for the selected altitude sectors varies between 0.428 and 0.824, indicating moderate to good agreement at all altitudes. GRASP shows denser aerosol layers in the mid-troposphere, while MERRA-2 gives higher aerosol extinctions throughout the high troposphere to low stratosphere region. Moreover, GRASP does not provide vertical variability in the extinction profile near the ground, due to a lack of data in the LIDAR’s incomplete overlap range. Lastly, the aerosol layer identification and type recognition are validated with statistical analysis of air mass backward trajectories with endpoints spatially and temporally collocated with individual identified layers. These reveal potential source regions that are located within areas known to be significant sources for the different identified aerosol types.

Arctic warming by abundant fine sea salt aerosols from blowing snow

The Arctic warms nearly four times faster than the global average, and aerosols play an increasingly important role in Arctic climate change. In the Arctic, sea salt is a major aerosol component in terms of mass concentration during winter and spring. However, the mechanisms of sea salt aerosol production remain unclear. Sea salt aerosols are typically thought to be relatively large in size but low in number concentration, implying that their influence on cloud condensation nuclei population and cloud properties is generally minor. Here we present observational evidence of abundant sea salt aerosol production from blowing snow in the central Arctic. Blowing snow was observed more than 20% of the time from November to April. The sublimation of blowing snow generates high concentrations of fine-mode sea salt aerosol (diameter below 300 nm), enhancing cloud condensation nuclei concentrations up to tenfold above background levels. Using a global chemical transport model, we estimate that from November to April north of 70° N, sea salt aerosol produced from blowing snow accounts for about 27.6% of the total particle number, and the sea salt aerosol increases the longwave emissivity of clouds, leading to a calculated surface warming of +2.30 W m−2 under cloudy sky conditions.

A review of recent research progress on the effect of external influences on tropical cyclone intensity change

Over the past four years, significant research has advanced our understanding of how external factors influence tropical cyclone (TC) intensity changes. Research on air-sea interactions shows that increasing the moisture disequilibrium is a very effective way to increase surface heat fluxes and that ocean salinity-stratification plays a non-negligible part in TC intensity change. Vertical wind shear from the environment induces vortex misalignment, which controls the onset of significant TC intensification. Blocking due to upper-level outflow from TCs can reduce the magnitude of vertical wind shear, making for TC intensification. Enhanced TC-trough interactions are vital for rapid intensification in some TC cases because of strengthened warm air advection, but upper-level troughs are found to limit TC intensification in other cases due to dry midlevel air intrusions and increased shear. Aerosol effects on TCs can be divided into direct effects involving aerosol-radiation interactions and indirect effects involving aerosol-cloud interactions. The radiation absorption by the aerosols can change the temperature profile and affect outer rainbands through changes in stability and microphysics. Sea spray and sea salt aerosols are more important in the inner region, where the aerosols increase precipitation and latent heating, promoting more intensification. For landfalling TCs, the intensity decay is initially more sensitive to surface roughness than soil moisture, and the subsequent decay is mainly due to the rapid reduction in surface moisture fluxes. These new insights further sharpen our understanding of the mechanisms by which external factors influence TC intensity changes.

Climatology of aerosol properties at an atmospheric monitoring site on the northern California coast

Abstract. Between April 2002 and June 2017, the Global Monitoring Laboratory (GML) of the National Oceanic and Atmospheric Administration (NOAA) made continuous measurements of a suite of in situ aerosol optical properties at a long-term monitoring site near Trinidad Head (THD), California. In addition to aerosol optical properties, between 2002–2006 a scanning humidograph system was operated, and inorganic ion and total aerosol mass concentrations were obtained from filter measurements. A combined analysis of these datasets demonstrates consistent patterns in aerosol climatology and highlights changes in sources throughout the year. THD is predictably dominated by sea salt aerosols; however, marine biogenic aerosols are the largest contributor to PM1 in the warmer months. Additionally, a persistent combustion source appears in the winter, likely a result of wintertime home heating. While the influences of local anthropogenic sources from vehicular and marine traffic are visible in the optical aerosol data, their influence is largely dictated by the wind direction at the site. Comparison of the THD aerosol climatology to that reported for other marine sites shows that the location is representative of clean marine measurements, even with the periodic influence of anthropogenic sources.

Fog and rain water chemistry in a tea plantation of northern Taiwan.

Tea plantations are expanding globally and many are in mountainous areas with frequent fog but few studies have examined fog chemistry in these areas. We examined chemical composition of fog and rain water at a tea plantation in northern Taiwan. Fog water was collected using a Kroneis passive cylindrical fog-water collector and rain water was collected using a 20-cm-diameter funnel. The most abundant ions were Cl- and Na+ in both fog and rain waters due to the proximity of the site to the coast. The order of abundance of other ions was NO3- > Mg2+ > SO42- > Ca2+ > NH4+ > K+ > H+ in fog water and SO42- > K+ > NO3- > NH4+ > Ca2+ > Mg2+ > H+ in rain water. The concentration enrichment ratio (fog to rain) ranged between 2.2 (K+) and 22 (Mg2+) lying between sites near major emission sources and sites in remote areas, possibly because the immediate surrounding landscape is covered with secondary forests although it is near large cities. Factor analysis highlights the influences of sea-salt aerosols on the variation of fog and rain water chemistry. Sea-salt corrections using Na+ as the sea salt tracer led to negative concentrations of Cl- and Mg2+ suggesting that assumptions involved in sea-salt corrections were not satisfied. Agriculture influence is identified as a unique factor for explaining variance of K+, NH4+, and dissolved organic nitrogen (DON) concentrations in fog water but not rain water. Ion concentrations in fog and rain water were generally higher in the weekly samples associated with air trajectories passing through the continental East Asia than those associated with oceanic trajectories pointing to the role of regional pollution sources in affecting local fog and rain water chemistry. Our study highlights greater effects of tea agriculture on fog than rain water chemistry.

Chemical processes of wintertime aerosols over the East China Sea based on aircraft and ground measurements: Comparison with the Sea of Japan

Aircraft and ground-level observations of wintertime aerosols over the East China Sea (ECS) around Japan's southwestern islands were conducted from the boundary layer to the middle troposphere (0–4.5 km) and compared to those over the Sea of Japan (SOJ) during the same period, for the purpose of comprehensive elucidation on modification process of chemical composition in aerosols at the Asian outflow receptor regions. The deficient values of Cl− in both cases for ECS and SOJ were higher at ground level than at high altitudes because of the acidic gas (HNO3, H2SO4) concentrations. Most Na+ and Cl− at high altitudes and at ground level originated from sea salt, because the (Na+ + Cl−) concentrations of which in the boundary layer observed were linearly related to the production flux of sea spray aerosol. The contribution of sea salt aerosols to cloud condensation nuclei appears to be low over the ECS, contrary to the SOJ. The non-sea salt (nss)-K+ concentrations and the path of backward trajectories suggest a significant impact of biomass burning on the SOJ associated with woodburning for residential heating in the Korean Peninsula. A similar difference was observed in NH4+/nss-SO42– equivalent ratios (∼0.5 for the ECS; ∼1 for the SOJ), which likely indicates ammonium sulfate aerosols produced in urban and industrial regions of Korea. The high aerosol Ca2+ concentration in the boundary layer over the ECS was accompanied by those of Na+, Cl−, NO3−, and nss-SO42– during cold front passages, as observed in SOJ. This indicates that Ca(NO3)2, CaSO4, and CaCl2 were formed via the reactions of acidic gases and Ca-rich dust particles from desert areas in the Asian continent, followed by the production of NaNO3 by uptake of acidic gases into sea salt in the ECS. This notion is supported by high Se(VI)/Se (IV) ratios (>2) that indicate an oxidative process during long-range transport from coal combustion sources.

Daytime Atmospheric Halogen Cycling through Aqueous-Phase Oxygen Atom Chemistry.

Halogen atoms are important atmospheric oxidants that have unidentified daytime sources from photochemical halide oxidation in sea salt aerosols. Here, we show that the photolysis of nitrate in aqueous chloride solutions generates nitryl chloride (ClNO2) in addition to Cl2 and HOCl. Experimental and modeling evidence suggests that O(3P) formed in the minor photolysis channel from nitrate oxidizes chloride to Cl2 and HOCl, which reacts with nitrite to form ClNO2. This chemistry is different than currently accepted mechanisms involving chloride oxidation by OH and could shift our understanding of daytime halogen cycling in the lower atmosphere.

Harmful algal bloom aerosols and human health.

Harmful algal blooms (HABs) are increasing across many locations globally. Toxins from HABs can be incorporated into aerosols and transported inland, where subsequent exposure and inhalation can induce adverse health effects. However, the relationship between HAB aerosols and health outcomes remains unclear despite the potential for population-level exposures. In this review, we synthesized the current state of knowledge and identified evidence gaps in the relationship between HAB aerosols and human health. Aerosols from Karenia brevis, Ostreopsis sp., and cyanobacteria were linked with respiratory outcomes. However, most works did not directly measure aerosol or toxin concentrations and instead relied on proxy metrics of exposure, such as cell concentrations in nearby waterbodies. Furthermore, the number of studies with epidemiological designs was limited. Significant uncertainties remain regarding the health effects of other HAB species; threshold dose and the dose-response relationship; effects of concurrent exposures to mixtures of toxins and other aerosol sources, such as microplastics and metals; the impact of long-term exposures; and disparities in exposures and associated health effects across potentially vulnerable subpopulations. Additional studies employing multifaceted exposure assessment methods and leveraging large health databases could address such gaps and improve our understanding of the public health burden of HABs.

Evaluation of lightning warning technique with multi-source data for Vung Tau coastal area

In this paper, the authors used multi-source data, including the electric field data observed by EFM-100C at Rescue Station No. 1 on the “Bai Sau” beach in Vung Tau coastal area for 166 days from May to October 2019; Himawari satellite data and Nha Be weather radar data and the GLD-360 lightning position data to evaluate the lightning warning method. Radar and satellite data were used to determine deep convective clouds. The GLD-360 lightning position data were used to examine the consistency of lightning location with the deep convective clouds. The “two areas” method was applied. The Area of Concern (AOC) has a radius of 10 km from the electric field measurement station. The Warning Area (WA) is 20 km extending from the outermost AOC area. Due to the influence of sea-salt aerosol on the background electric field intensity, the electric field threshold selected for a warning is larger than the absolute value (1.5 kV/m). The results showed that the probability of detection (POD), failure to warn (FTW), and false alarm ratio (FAR) were 86.3%, 13.07%, and 23.17%, respectively. The average time of lightning warning for the Vung Tau coastal area is 23 minutes in advance. The warning time is equivalent to that in some studies around the world. The value is suitable for practical application in lightning prevention on the beach and in the Vung Tau coastal area.

Modeling atmospheric microplastic cycle by GEOS-Chem: An optimized estimation by a global dataset suggests likely 50 times lower ocean emissions

Modeling atmospheric microplastic cycle by GEOS-Chem: An optimized estimation by a global dataset suggests likely 50 times lower ocean emissions

Cyclones enhance the transport of sea salt aerosols to the high atmosphere in the Southern Ocean

Cyclones enhance the transport of sea salt aerosols to the high atmosphere in the Southern Ocean

Technical note: Sublimation of frozen CsCl solutions in an environmental scanning electron microscope (ESEM) – determining the number and size of salt particles relevant to sea salt aerosols

Abstract. We present a novel technique that elucidates the mechanism of the formation of small aerosolizable salt particles from salty frozen samples. We demonstrated that CsCl may be a suitable probe for sea salts due to its similar subzero properties and sublimation outcomes: CsCl substantially increased the visibility of the salt both during and after ice sublimation. Hence, we identified the factors that, during the sublimation of a frozen salty solution, are important in generating fine salt particles as a possible source of salt aerosol. The number, size, and structure of the particles that remain after ice sublimation were investigated with respect to the concentration of the salt in the sample, the freezing method, and the sublimation temperature. The last-named aspect is evidently of primary importance for the preference of fine salt crystals over a large compact piece of salt; we showed that the formation of small salt particles is generally restricted if the brine is liquid during the ice sublimation, i.e. at temperatures higher than the eutectic temperature (Teu). Small salt particles that might be a source of atmospheric aerosols were formed predominantly at temperatures below Teu, and their structures strongly depended on the concentration of the salt. For example, the sublimation of those samples that exhibited a concentration of less than 0.05 M often produced small aerosolizable isolated particles that are readily able to be windblown. Conversely, the sublimation of 0.5 M samples led to the formation of relatively stable and largely interconnected salt structures. Our findings are in good agreement with other laboratory studies which have unsuccessfully sought salt aerosols from, for example, frost flowers at temperatures above Teu. This study offers an explanation of the previously unexplored behaviour.

Ionic Strength Enhances the Multiphase Oxidation Rate of Sulfur Dioxide by Ozone in Aqueous Aerosols: Implications for Sulfate Production in the Marine Atmosphere.

Multiphase oxidation of sulfur dioxide (SO2) by ozone (O3) in alkaline sea salt aerosols is an important source of sulfate aerosols in the marine atmosphere. However, a recently reported low pH of fresh supermicron sea spray aerosols (mainly sea salt) would argue against the importance of this mechanism. Here, we investigated the impact of ionic strength on the kinetics of multiphase oxidation of SO2 by O3 in proxies of aqueous acidified sea salt aerosols with buffered pH of ∼4.0 via well-controlled flow tube experiments. We find that the sulfate formation rate for the O3 oxidation pathway proceeds 7.9 to 233 times faster under high ionic strength conditions of 2-14 mol kg-1 compared to the dilute bulk solutions. The ionic strength effect is likely to sustain the importance of multiphase oxidation of SO2 by O3 in sea salt aerosols in the marine atmosphere. Our results indicate that atmospheric models should consider the ionic strength effects on the multiphase oxidation of SO2 by O3 in sea salt aerosols to improve the predictions of the sulfate formation rate and the sulfate aerosol budget in the marine atmosphere.