Sea-salt Aerosol Particles Research Articles

Polarization characterization of a nonspherical sea salt aerosol model

The T-matrix method was utilized to study the polarization characteristics of nonspherical sea salt aerosol models within the wavelength range of 0.48–2.5 µm. Analysis was conducted on the polarization characteristics of nonspherical sea salt aerosols across different wavelengths as a function of scattering angle. This included scrutinizing linear depolarization ratios under typical visible and near-infrared wavelengths for various aspect ratios. The impact of particle nonsphericity on the linear depolarization ratios of monodisperse and polydisperse sea salt aerosol particles was examined. The results indicate: (1) In the analysis of the polarization characteristics of sea salt aerosols, the trends of polarization properties are similar between monodisperse and polydisperse systems. The scattering phase function P11(θ) is predominantly more significant in the forward-scattering direction. P11(θ) is insensitive to wavelength changes in the backward-scattering direction. P33(θ)/P11(θ) varies across different bands; in the visible light spectrum, there are significant fluctuating changes, while in the infrared spectrum, it trends towards nearly linear changes. The variation trends of −P12(θ)/P11(θ) and P34(θ)/P11(θ) with scattering angle are similar, and both are significantly affected by changes in wavelength. (2) Regarding the depolarization ratio of sea salt aerosols, the value for polydisperse systems is more than twice that of monodisperse systems, and the greater the nonsphericity, the higher the linear depolarization ratio. In monodisperse systems, at a wavelength of 0.633 µm for visible light and an aspect ratio of 0.4, the maximum depolarization ratio is around 118.82, while at 1.65 µm in the near-infrared, with an aspect ratio of 0.2, the maximum depolarization ratio is near 97.52; under polydisperse conditions, at 0.633 µm for visible light and an aspect ratio of 0.4, the maximum depolarization ratio is around 117.18, while at 1.65 µm in the near-infrared, with an aspect ratio of 0.2, the maximum linear depolarization ratio is near 215.66. Investigating the polarization characteristics and linear depolarization ratios of nonspherical spheroid sea salt aerosol particle models at all scattering angles is important for remote-sensing detection, high-precision calibration, and other optoelectronic applications.

Investigation of Light-Scattering Properties of Non-Spherical Sea Salt Aerosol Particles at Varying Levels of Relative Humidity

In the marine environment, sea salt aerosol particles transition from cubic or rectangular shapes when dry to various non-spherical shapes like ellipsoids and cylinders under different humidities. The complex humidity conditions and particle morphologies pose challenges to simulating the optical scattering properties of non-spherical sea salt aerosols. This study, addressing real environmental scenarios, employs the randomly oriented T-matrix computational method to calculate the optical scattering and polarization characteristics of sea salt aerosols at a wavelength of 1.06 μm under three relative humidity conditions (50%, 80%, and 95%) and three particle morphologies (spheroid, circular cylinder, and Chebyshev particle shapes). The results show the following: (1) In terms of optical scattering properties, the greater the non-sphericity of particles under the same humidity conditions, the larger the deviation between non-spherical and spherical models. For spheroid and circular cylinder sea salt aerosols, the error in the extinction efficiency factor mainly lies within 10–30%, reaching up to 120%; the error in the asymmetry factor is primarily between 3 and 25%, with a maximum of 75%, and the error in the forward-scattering phase function is mainly within 10–60%, reaching up to 180%. Chebyshev particle-shaped sea salt aerosols exhibit smaller deviations in optical scattering properties compared to equivalent spherical models, generally within the 5–25% range. Under different humidity conditions, the scattering characteristic parameters of sea salt aerosol particles for various non-spherical models show a positive correlation with relative humidity. When relative humidity is below 70%, the optical scattering properties of differently shaped sea salt aerosols are less affected by relative humidity. Above 70% relative humidity, the optical scattering properties of sea salt aerosols of different shapes become more sensitive to changes in relative humidity. (2) Regarding polarization properties, the greater the humidity, the more significant the impact on polarization properties, and as humidity increases, sea salt aerosols with higher non-sphericity exhibit more complex changes in polarization characteristics. The differences in shapes of non-spherical models mainly affect the numerical values of polarization properties. Under the same humidity conditions, spheroid polarization characteristics are significantly different from other models. In terms of depolarization ratio for aerosols, circular cylinder sea salt aerosols show the highest depolarization ratio at various relative humidities, followed by spheroid, with Chebyshev-shaped having the least. The effect of relative humidity on the depolarization ratio varies with the scattering angle. The higher the relative humidity, the more complex the variation in the depolarization ratio with scattering angle, with more pronounced oscillations in the curve, and the less non-spherical the shape, the more intense the oscillations in the depolarization ratio curve due to humidity. In conclusion, this study calculated the optical scattering and polarization properties of sea salt aerosol particles under different relative humidities and shapes, which is of significant importance for applications like 1.06 μm laser engineering and atmospheric radiation transmission in actual marine scenarios.

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.

Missed Evaporation from Atmospherically Relevant Inorganic Mixtures Confounds Experimental Aerosol Studies.

Sea salt aerosol particles are highly abundant in the atmosphere and play important roles in the global radiative balance. After influence from continental air, they are typically composed of Na+, Cl-, NH4+, and SO42- and organics. Analogous particle systems are often studied in laboratory settings by atomizing and drying particles from a solution. Here, we present evidence that such laboratory studies may be consistently biased in that they neglect losses of solutes to the gas phase. We present experimental evidence from a hygroscopic tandem differential mobility analyzer and an aerosol mass spectrometer, further supported by thermodynamic modeling. We show that, at normally prevailing laboratory aerosol mass concentrations, for mixtures of NaCl and (NH4)2SO4, a significant portion of the Cl- and NH4+ ions are lost to the gas phase, in some cases, leaving mainly Na2SO4 in the dry particles. Not considering losses of solutes to the gas phase during experimental studies will likely result in misinterpretation of the data. One example of such data is that from particle water uptake experiments. This may bias the explanatory models constructed from the data and introduce errors inte predictions made by air quality or climate models.

Hygroscopic growth of single atmospheric sea salt aerosol particles from mass measurement in an optical trap.

Sea salt aerosol is among the most abundant aerosol species in Earth's atmosphere, and its hygroscopicity is an important parameter to quantify its interaction with solar radiation. Conflicting values for the hygroscopic growth have been reported in the literature, which decreases the accuracy with which their impact on Earth's climate can be modelled. Here we report new values of the hygroscopic growth for a selection of salt compositions representative of atmospheric sea salt. These values are obtained from single optically trapped aqueous droplets with dry radii between 0.3 and 2 μm, using a recently developed method for single particle mass measurement in an optical trap. We compare our results to earlier studies and propose a way to reconcile the apparent discrepancies found in the literature. Within our studies, we also observe the crystallization of CaSO4·2H2O (Gypsum) during the drying of optically trapped sea salt droplets at significantly larger relative humidity of 65-68% than the main efflorescence relative humidity at 50%. This preceding transition occurred in the absence of any contact of the particle with a surface.

A Parameterization of Interstitial Aerosol Extinction and Its Application to Marine Cloud Brightening

Abstract Marine cloud brightening (MCB) is a geoengineering approach to counteract climate change by the deliberate seeding of sea salt aerosol particles that, once they activated to cloud droplets, directly increase cloud reflectance and hence global albedo. However, a large fraction of the seeded aerosol may remain interstitial, i.e., unactivated particles among cloud droplets. Because the consideration of interstitial aerosol optical properties usually requires computationally expensive simulations of the entire particle spectrum and direct Mie calculations, we develop a simple parameterization to be used with computationally efficient bulk and even bin cloud microphysical schemes that do not treat the unactivated aerosol explicitly. Using parcel and large-eddy simulations with highly detailed Lagrangian cloud microphysics and direct Mie calculations as a reference, we show that the parameterization captures the variability in the interstitial aerosol extinction successfully. By applying the parameterization to typical MCB cases, we find that the consideration of interstitial aerosol extinction is important for the assessment of MCB in shallow clouds with weak updrafts, in which only a small fraction of aerosol particles is activated to cloud droplets. Significance Statement The optical properties of clouds are not only determined by the number and size of cloud droplets. Unactivated aerosol particles, so-called interstitial aerosol, can contribute substantially to the optical thickness of shallow clouds with weak updrafts in aerosol-laden conditions. The consideration of interstitial aerosol optical thickness has been computationally challenging, but the new parameterization presented here allows for an efficient representation in various types of cloud models. The parameterization is shown to be an important addition for the assessment of marine cloud brightening (MCB), a potential geoengineering technique to counteract global warming by increasing the cloud albedo through the deliberate seeding of aerosol.

Numerical Investigation on the Atomization Characteristics of An Aerosol Spray Nozzle

Inlet air filtration of ships and coastal installations is mainly used to filter out salt aerosol particles, so researches on the inlet filter needs to simulate spray aerosol state in the marine environment. The sea salt aerosol particles have multiple sizes, thus salt aerosol generator should have the ability to produce salt aerosol particles of various diameters. This paper investigates the factors that affect the particle diameter of a salt aerosol generating device. Numerical simulations on the two-phase flow in a salt aerosol nozzle are conducted and the influence of air inlet pressure and droplet mass flow rate on the particle diameter is discovered. The results show that the particle diameter of the aerosol nozzle decreases with the air inlet pressure increasing and the droplet mass flow rate decreasing.

Changes in aerosol particle composition during sea fog formation events in the sea ice regions of the Arctic Ocean

Water soluble ions (WSIs) of aerosol particles is one of the important parameters to study the aerosol-fog interactions. To study the changes of aerosol WSIs during sea fog events, hourly real-time measurements of WSIs (Na+, K+, Mg2+, Ca2+, MSA−, Cl−, NO3−, and SO42−) in total suspended aerosol particles (TSP) were conducted in the atmosphere over Arctic Ocean ice floe regions from August 1 to 12, 2017, when the sea fog events were frequently observed. There were significant differences in Na+, Cl−, Mg2+, methanesulfonic acid (MSA−), sea salt sulfate (ss-SO42) and non-sea salt sulfate (nss-SO42-) ions during sea fog events vs. non-sea fog periods. The mass concentrations of sea salt ions, such as Na+, Mg2+, Cl− and ss-SO42-, clearly increased before the occurrence of sea fog and then decreased substantially with the formation of sea fog; however, nss-SO42- levels did not decrease but remained high during the sea fog processes. These results suggest that sea salt aerosol particles were more likely to serve as condensation nuclei for fog and could be more effectively removed by sea fog than nss-SO42- particles. MSA− only combined with sea salt particles, which were likely to serve as condensation nuclei and be removed by sea fog. Condensation may be the primary factor leading to the reduction of sea salt ions during the sea fog periods, while other factors like the presence of dense sea ice and long-range transport input may also affect the decreasing rate.

Surface composition of size-selected sea salt particles under the influence of organic acids studied in situ using synchrotron radiation X-ray photoelectron spectroscopy

Synchrotron X-ray photoelectron spectroscopic surface characterisation of size-resolved sea salt aerosol particles revealed Mg enrichment in the particle surface layer which was either enhanced or decreased depending on the organic compound added.

Modelling effects of alkylamines on sea salt aerosols using the Extended Aerosols and Inorganics Model

Sea salt aerosols are known to serve as effective cloud condensation nuclei and are prominent contributors of light scattering in the atmosphere. More light scattering reduces solar radiations to the Earth and lowers the global temperature. Researchers observed that ambient sea salt aerosols may contain ammonium sulfate (AS) and sodium chloride (NaCl). Recent studies showed that alkylamines, derivatives of ammonia, can react with ammonium salts in the aerosol, displacing ammonium and altering the particle’s properties. Our study investigated the effects of atmospheric alkylamines on the properties of sea salt aerosols using a chemical system of methylamine (MA), AS, and NaCl. We determined the relative humidity when these aerosols start to absorb water vapor from the air (deliquescent relative humidity, DRH), and concentrations of ammonia and MA in aqueous/gas phases using the Extended Aerosols and Inorganics Model. Our findings indicate a notable negative relationship between MA concentration and the DRH for both AS and NaCl. We determined that five parts per billion or higher of MA effectively lowered the DRH of sea salt aerosol particles. The concentrations of ammonia and MA in aqueous and gas phases had a complex dependence on MA concentration and aerosol chemical composition. Aerosol deliquescence often leads to cloud/fog processing which may cool the Earth by reflecting sunlight away from the surface. Therefore, our results implicate a potential role for alkylamines in climate change, suggesting the importance of monitoring alkylamine concentrations in the atmosphere. Future studies are needed to better predict the deliquescent behaviors of aerosols, namely particles containing AS and NaCl, such as those found near coasts.

Long-range transport of anthropogenic air pollutants into the marine air: insight into fine particle transport and chloride depletion on sea salts

Abstract. Long-range transport of anthropogenic air pollutants from East Asia can affect the downwind marine air quality during spring and winter. Long-range transport of continental air pollutants and their interaction with sea salt aerosol (SSA) significantly modify the radiative forcing of marine aerosols and influence ocean biogeochemical cycling. Previous studies poorly characterize variations of aerosol particles along with air mass transport from the continental edge to the remote ocean. Here, the research ship R/V Dongfanghong 2 traveled from the eastern China seas (ECS) to the northwestern Pacific Ocean (NWPO) to understand what and how air pollutants were transported from the highly polluted continental air to clean marine air in spring. A transmission electron microscope (TEM) was used to find the long-range transported anthropogenic particles and the possible Cl-depletion phenomenon of SSA in marine air. Anthropogenic aerosols (e.g., sulfur (S)-rich, S-soot, S-metal/fly ash, organic matter (OM)-S, and OM coating particles) were identified and dramatically declined from 87 % to 8 % by number from the ECS to remote NWPO. For the SSA aging, 87 % of SSA particles in the ECS were identified as fully aged, while the proportion of fully aged SSA particles in the NWPO decreased to 29 %. Our results highlight that anthropogenic acidic gases in the troposphere (e.g., SO2, NOx, and volatile organic compounds) could be transported to remote marine air and exert a significant impact on aging of SSA particles in the NWPO. The study shows that anthropogenic particles and gases from East Asia significantly perturb different aerosol chemistry from coastal to remote marine air. More attention should be given to the modification of SSA particles in remote marine areas due to the influence of anthropogenic gaseous pollutants.

Modeling the Aerosol Extinction in Marine and Coastal Areas

Sea salt aerosol (SSA) significantly affects the atmospheric albedo, the radiation balance of the Earth, and has consequences for global and regional climate. There is currently no reliable radiative large-scale aerosol model of the marine and coastal atmosphere. All these lead to uncertainties in radiation boxes, short-term weather forecasts, and climate models and to uncertainties in interpretation of the lidar return data obtained and at the development of new lidar systems. The MaexPro model is shown to calculate adequately the aerosol extinction coefficients $\varepsilon (\lambda)$ and the concentration of SSA particles for different wind regimes, fetches, and humidity. The calculated $\varepsilon (\lambda)$ profiles well agree with the experimental data and with calculations using Advanced Navy Aerosol Model (ANAM) and MODTRAN codes. A new approach in studying the influence of the meteorological parameters on spectral $\varepsilon (\lambda)$ gives a new explanation for previously obtained conflicting experimental data, namely, to the effect of decreasing transparency, manifested in the coastal zone, and makes it possible indirectly to account for the type of air mass (marine or coastal). It is shown that the particle size distribution functions and spectral $\varepsilon (\lambda)$ , calculated using the model with the input parameters corresponding most closely to the conditions of experiment, agree well with observations, using OLAF transmissometer, and calculations using MODTRAN code and the experimental results receiving the same conditions of observations (numerical or field). The results obtained are of interest both in the calculations of radiative characteristics of the atmosphere and in interpretation of the lidar return data and calibration signal when developing new lidar systems.

Halogen activation and radical cycling initiated by imidazole-2-carboxaldehyde photochemistry

Abstract. Atmospheric aerosol particles can contain light-absorbing organic compounds, also referred to as brown carbon (BrC). The ocean surface and sea spray aerosol particles can also contain light-absorbing organic species referred to as chromophoric dissolved organic matter (CDOM). Many BrC and CDOM species can contain carbonyls, dicarbonyls or aromatic carbonyls such as imidazole-2-carboxaldehyde (IC), which may act as photosensitizers because they form triplet excited states upon UV–VIS light absorption. These triplet excited states are strong oxidants and may initiate catalytic radical reaction cycles within and at the surface of atmospheric aerosol particles, thereby increasing the production of condensed-phase reactive oxygen species (ROS). Triplet states or ROS can also react with halides, generating halogen radicals and molecular halogen compounds. In particular, molecular halogens can be released into the gas phase, which is one halogen activation pathway. In this work, we studied the influence of bromide and iodide on the photosensitized production and release of hydroperoxy radicals (HO2) upon UV irradiation of films in a coated wall flow tube (CWFT) containing IC in a matrix of citric acid (CA) irradiated with UV light. In addition, we measured the iodine release upon irradiation of IC ∕ CA films in the CWFT. We developed a kinetic model coupling photosensitized CA oxidation with condensed-phase halogen chemistry to support data analysis and assessment of atmospheric implications in terms of HO2 production and halogen release in sea spray particles. As indicated by the experimental results and confirmed by the model, significant recycling of halogen species occurred via scavenging reactions with HO2. These prevented the full and immediate release of the molecular halogen (bromine and iodine) produced. Recycling was stronger at low relative humidity, attributed to diffusion limitations. Our findings also show that the HO2 production from BrC or CDOM photosensitized reactions can increase due to the presence of halides, leading to high HO2 turnover, in spite of low release due to the scavenging reactions. We estimated the iodine production within sea salt aerosol particles due to iodide oxidation by ozone (O3) at 5.0×10-6 M s−1 assuming O3 was in Henry's law equilibrium with the particle. However, using an O3 diffusion coefficient of 1×10-12 cm2 s−1, iodine activation in an aged, organic-rich sea spray is estimated to be 5.5×10-8 M s−1. The estimated iodine production from BrC photochemistry based on the results reported here amounts to 4.1×10-7 M s−1 and indicates that BrC photochemistry can exceed O3 reactive uptake in controlling the rates of iodine activation from sea spray particles under dry or cold conditions where diffusion is slow within particles.

CCN measurements at the Princess Elisabeth Antarctica research station during three austral summers

Abstract. For three austral summer seasons (2013–2016, each from December to February) aerosol particles arriving at the Belgian Antarctic research station Princess Elisabeth (PE) in Dronning Maud Land in East Antarctica were characterized. This included number concentrations of total aerosol particles (NCN) and cloud condensation nuclei (NCCN), the particle number size distribution (PNSD), the aerosol particle hygroscopicity, and the influence of the air mass origin on NCN and NCCN. In general NCN was found to range from 40 to 6700 cm−3, with a median of 333 cm−3, while NCCN was found to cover a range between less than 10 and 1300 cm−3 for supersaturations (SSs) between 0.1 % and 0.7 %. It is shown that the aerosol is dominated by the Aitken mode, being characterized by a significant amount of small, and therefore likely secondarily formed, aerosol particles, with 94 % and 36 % of the aerosol particles smaller than 90 and ≈35 nm, respectively. Measurements of the basic meteorological parameters as well as the history of the air masses arriving at the measurement station indicate that the station is influenced by both marine air masses originating from the Southern Ocean and coastal areas around Antarctica (marine events – MEs) and continental air masses (continental events – CEs). CEs, which were defined as instances when the air masses spent at least 90 % of the time over the Antarctic continent during the last 10 days prior to arrival at the measurements station, occurred during 61 % of the time during which measurements were done. CEs came along with rather constant NCN and NCCN values, which we denote as Antarctic continental background concentrations. MEs, however, cause large fluctuations in NCN and NCCN, with low concentrations likely caused by scavenging due to precipitation and high concentrations likely originating from new particle formation (NPF) based on marine precursors. The application of HYSPLIT back trajectories in form of the potential source contribution function (PSCF) analysis indicate that the region of the Southern Ocean is a potential source of Aitken mode particles. On the basis of PNSDs, together with NCCN measured at an SS of 0.1 %, median values for the critical diameter for cloud droplet activation and the aerosol particle hygroscopicity parameter κ were determined to be 110 nm and 1, respectively. For particles larger than ≈110 nm the Southern Ocean together with parts of the Antarctic ice shelf regions were found to be potential source regions. While the former may contribute sea spray particles directly, the contribution of the latter may be due to the emission of sea salt aerosol particles, released from snow particles from surface snow layers, e.g., during periods of high wind speed, leading to drifting or blowing snow. The region of the Antarctic inland plateau, however, was not found to feature a significant source region for aerosol particles in general or for cloud condensation nuclei measured at the PE station in the austral summer.

Heterogeneous Ice Nucleation Ability of NaCl and Sea Salt Aerosol Particles at Cirrus Temperatures

AbstractIn situ measurements of the composition of heterogeneous cirrus ice cloud residuals have indicated a substantial contribution of sea salt in sampling regions above the ocean. We have investigated the heterogeneous ice nucleation ability of sodium chloride (NaCl) and sea salt aerosol (SSA) particles at cirrus cloud temperatures between 235 and 200 K in the Aerosol Interaction and Dynamics in the Atmosphere aerosol and cloud chamber. Effloresced NaCl particles were found to act as ice nucleating particles in the deposition nucleation mode at temperatures below about 225 K, with freezing onsets in terms of the ice saturation ratio, Sice, between 1.28 and 1.40. Above 225 K, the crystalline NaCl particles deliquesced and nucleated ice homogeneously. The heterogeneous ice nucleation efficiency was rather similar for the two crystalline forms of NaCl (anhydrous NaCl and NaCl dihydrate). Mixed‐phase (solid/liquid) SSA particles were found to act as ice nucleating particles in the immersion freezing mode at temperatures below about 220 K, with freezing onsets in terms of Sice between 1.24 and 1.42. Above 220 K, the SSA particles fully deliquesced and nucleated ice homogeneously. Ice nucleation active surface site densities of the SSA particles were found to be in the range between 1.0 · 1010 and 1.0 · 1011 m−2 at T < 220 K. These values are of the same order of magnitude as ice nucleation active surface site densities recently determined for desert dust, suggesting a potential contribution of SSA particles to low‐temperature heterogeneous ice nucleation in the atmosphere.

Condensational Growth of Drops Formed on Giant Sea-Salt Aerosol Particles

Abstract The most basic aspect of cloud formation is condensational growth onto cloud condensation nuclei (CCN). As such, condensational growth of cloud drops is often assumed to be a well-understood process described by the drop growth equation. When this process is represented in models, CCN activate into cloud drops at cloud base, and it is often assumed that drops consist of pure water or that the hygroscopic contribution after drop activation is small because of the inclusion of only small CCN. Drop growth rate in adiabatic ascent in such models is proportional to supersaturation and assumed to be inversely proportional to the drop radius, thereby making the drop spectrum narrow with altitude. However, the present study demonstrates that drop growth on giant sea-salt aerosol particles (GCCN; dry radius 0.5 m) behaves differently. For typical marine stratocumulus updrafts and for drops grown on GCCN with sizes m, these drops typically remain concentrated salt solutions. Because of this, their condensational growth is accelerated, and they rapidly attain precipitation drop sizes through condensation only. Additionally, drops formed on GCCN may also grow by condensation in cloudy downdrafts. The strong effect of condensation on GCCN is important when carried through to calculating rain-rate contribution as a function of aerosol size. GCCN larger than 2 m account for most of the rainfall rate in the modeled precipitating marine stratocumulus.

Temperature-dependent formation of NaCl dihydrate in levitated NaCl and sea salt aerosol particles.

Recent laboratory studies indicate that the hydrated form of crystalline NaCl is potentially important for atmospheric processes involving depositional ice nucleation on NaCl dihydrate particles under cirrus cloud conditions. However, recent experimental studies reported a strong discrepancy between the temperature intervals where the efflorescence of NaCl dihydrate has been observed. Here we report the measurements of the volume specific nucleation rate of crystalline NaCl in the aqueous solution droplets of pure NaCl suspended in an electrodynamic balance at constant temperature and humidity in the range from 250 K to 241 K. Based on these measurements, we derive the interfacial energy of crystalline NaCl dihydrate in a supersaturated NaCl solution and determined its temperature dependence. Taking into account both temperature and concentration dependence of nucleation rate coefficients, we explain the difference in the observed fractions of NaCl dihydrate reported in the previous studies. Applying the heterogeneous classical nucleation theory model, we have been able to reproduce the 5 K shift of the NaCl dihydrate efflorescence curve observed for the sea salt aerosol particles, assuming the presence of super-micron solid inclusions (hypothetically gypsum or hemihydrate of CaSO4). These results support the notion that the phase transitions in microscopic droplets of supersaturated solution should be interpreted by accounting for the stochastic nature of homogeneous and heterogeneous nucleation and cannot be understood on the ground of bulk phase diagrams alone.

Sea salt aerosol deposition in the coastal zone: A large eddy simulation study

Inland deposition of sea salt aerosol (SSA) particles emitted over the ocean is studied via numerical and theoretical models. The focus is on the large particles that contribute most to the total mass deposition. Large eddy simulations of idealized sea wind are used to investigate the development of the particle plume over land for different particle sizes and to validate some of the assumptions in the theoretical model. An existing theoretical modeling framework for particle dispersion in the atmospheric boundary layer is adapted to the problem of SSA deposition and it is shown to be adequate for the large particles of interest here. The decay of monodisperse SSA particle deposition flux with distance from the shoreline is shown to have a power-law behavior far from the shoreline. A complete model for predicting mass deposition as a function of distance is formulated and shown to present reasonable agreement with existing data.

Hygroscopic properties of NaCl and NaNO<sub>3</sub> mixture particles as reacted inorganic sea-salt aerosol surrogates

Abstract. NaCl in fresh sea-salt aerosol (SSA) particles can partially or fully react with atmospheric NOx/HNO3, so internally mixed NaCl and NaNO3 aerosol particles can co-exist over a wide range of mixing ratios. Laboratory-generated, micrometer-sized NaCl and NaNO3 mixture particles at 10 mixing ratios (mole fractions of NaCl (XNaCl) = 0.1 to 0.9) were examined systematically to observe their hygroscopic behavior, derive experimental phase diagrams for deliquescence and efflorescence, and understand the efflorescence mechanism. During the humidifying process, aerosol particles with the eutonic composition (XNaCl = 0.38) showed only one phase transition at their mutual deliquescence relative humidity (MDRH) of 67.9 (±0.5)% On the other hand, particles with other mixing ratios showed two distinct deliquescence transitions; i.e., the eutonic component dissolved at MDRH, and the remainder in the solid phase dissolved completely at their DRHs depending on the mixing ratios, resulting in a phase diagram composed of four different phases, as predicted thermodynamically. During the dehydration process, NaCl-rich particles (XNaCl > 0.38) showed a two stage efflorescence transition: the first stage was purely driven by the homogeneous nucleation of NaCl and the second stage at the mutual efflorescence RH (MERH) of the eutonic components, with values in the range of 30.0–35.5%. Interestingly, aerosol particles with the eutonic composition (XNaCl = 0.38) also showed two-stage efflorescence, with NaCl crystallizing first followed by heterogeneous nucleation of the remaining NaNO3 on the NaCl seeds. NaNO3-rich particles (XNaCl ≤ 0.3) underwent single-stage efflorescence transitions at ERHs progressively lower than the MERH because of the homogeneous nucleation of NaCl and the almost simultaneous heterogeneous nucleation of NaNO3 on the NaCl seeds. SEM/EDX elemental mapping indicated that the effloresced NaCl–NaNO3 particles at all mixing ratios were composed of a homogeneously crystallized NaCl moiety in the center, surrounded either by the eutonic component (for XNaCl > 0.38) or NaNO3 (for XNaCl ≤ 0.38). During the humidifying or dehydration process, the amount of eutonic composed part drives particle/droplet growth or shrinkage at the MDRH or MERH (second ERH), respectively, and the amount of pure salts (NaCl or NaNO3 in NaCl- or NaNO3-rich particles, respectively) drives the second DRHs or first ERHs, respectively. Therefore, their behavior can be a precursor to the optical properties and direct radiative forcing for these atmospherically relevant mixture particles representing the coarse, reacted inorganic SSAs. In addition, the NaCl–NaNO3 mixture aerosol particles can maintain an aqueous phase over a wider RH range than pure NaCl particles as SSA surrogate, making their heterogeneous chemistry more probable.

Influence of Concentrations Dried Sea Salt Aerosols to Decrease Solar Radiation

The study was aimed to study influent concentration of total dried sea salt aerosol to decrease solar radiation located in Phetchaburi province by measuring wave-length between 300-1050 nm using spectroradiometer and model MS-700.Spearman,s correlation was used to determine the relationship between the different concentration of sea salt and the measurement of solar radiation. The result showed that decreasing percentage of solar radiation was decreased causing the reflection of radiation from the sun. Moreover high concentration of solar radiation from spectrum between 390-400 nm by small sea salt aerosol and soil particle. Radiation from the sun with wave-length (visible-light 400-700 nm) was increased due to size of soil particle and sea salt aerosol were smaller than the size of the wave-length. Radiation from the sun with wave-length (infrared 700-1040 nm) was increased in both sea salt aerosol and soil particle because the size of sea salt and soil particle were smaller than wave-length .The higher concentration of the sun concentration was in the wave-length between 910-930 nm and wave-length between 955-961 nm both in sea salt aerosol and soil particle. In additionally there should be a reduction of solar radiation in the wave-length between 955-961 nm. Which occurred only in sea salt aerosol due to radiation blocking (Chunkao, 1979) by sea salt particle. Radiation from the sun with wave-length between 1090-1120 nm was decreased the wave-length called atmospheric windrow, the sun radiation can be increased and decreased .Additionally the result showed correlations significant in wave-length 300-311,751-781,911-971 nm and significant high particular in wave-length 1070-1131 nm .respectively.