Hygroscopic growth of aerosol particles and its influence on nucleation scavenging in cloud: Experimental results from Kleiner Feldberg

The hygroscopic growth of individual aerosol particles has been measured with a Tandem Differential Mobility Analyser. The hygroscopic growth spectra were analysed in terms of diameter change with increasing RH from 20% to 85%. The measurements were carried out during the GCE cloud experiment at Kleiner Feldberg, Taunus, Germany in October and November 1990.Two groups of particles with different hygroscopic growth were observed. The less-hygroscopic group had average growth factors of 1.11, 1.04 and 1.02 for particle diameters of 50, 150 and 300 nm, respectively. The more-hygroscopic group had average growth factors of 1.34, 1.34, and 1.37 for the same particle diameters. The average fraction of less-hygroscopic particles was about 50%. Estimates of the soluble fractions of the particles belonging to the two groups are reported.Hygroscopic growth spectra for total aerosol, interstitial aerosol and cloud drop residuals were measured. A comparison of these hygroscopic growths of individual aerosol particles provides clear evidence for the importance of hygroscopic growth in nucleation scavenging. The measured scavenged fraction of particles as a function of diameter can be explained by the hygroscopic growth spectra.     

Simulation of rocket seeding of convective clouds with coarse-dispersion hygroscopic aerosol. 1. Condensational growth of the cloud droplets at the salt crystals

Patterns of propagation of aerosol particles generated in the hygroscopic seeding of convective clouds from antihail rockets is studied. Effects of the salt particle dispersity on condensational growth rate of separate cloud droplets on these particles are studied; analytical formulas are obtained as describing change of radius of the NaCl crystal and of the cloud droplet which grows on the crystal till the moment of full dissolving of the crystal in the droplet. Numerical computations are used for comparative analysis of the salt effect on intensification of condensational growth of the droplets in the cloud.     

Measurement of Ambient,Interstitial, and Residual Aerosol Particles on a Mountaintop Site in Central Sweden using an Aerosol Mass Spectrometer and a CVI

The Aerodyne aerosol mass spectrometer (Q-AMS) was coupled with a counterflow virtual impactor (CVI) for the first time to measure cloud droplet residuals of warm tropospheric clouds on Mt. Åreskutan in central Sweden in July 2003. Operating the CVI in different operational modes generated mass concentration and species-resolved mass distribution data for non-refractory species of the ambient, interstitial, and residual aerosol. The ambient aerosol measurements revealed that the aerosol at the site was mainly influenced by long-range transport and regional photochemical generation of nitrate and organic aerosol components. Four different major air masses were identified for the time interval of the experiment. While two air masses that approached the site from northeastern Europe via Finland showed very similar aerosol composition, the other two air masses from polar regions and the British Islands had a significantly different composition. During cloud events the larger aerosol particles were found to be activated into cloud droplets. On a mass basis the activation cut-off diameter was approximately 150 nm for nitrate and organics dominated particles and 200 nm for sulfate dominated particles. Generally nitrate and organics were found to be activated into cloud droplets with higher efficiency than sulfate. While a significant fraction of the nitrate in ambient particles was organic nitrates or nitrogen-containing organic species, the nitrate found in the cloud droplet residuals was mainly ammonium nitrate. After passage of clouds the ambient aerosol size distribution had shifted to smaller particle sizes due to the predominantly activation of larger aerosol particles without a significant change in the relative composition of the ambient aerosol.     

Simulation of rocket seeding of convective clouds with coarse-dispersion hygroscopic aerosol. 2. Condensation and coagulation in a cloud seeded with hygroscopic particles

A set of equations is developed to describe changes in cloud dispersity due to condensation and gravitational coagulation in the area of the salt particle diffusion in hygroscopic seeding of convective clouds with antihail rockets. Competition for moisture between the natural cloud droplets, entrained in the area from outside by turbulent diffusion, and artificial NaCl particles is taken into account. Optimum versions of hygroscopic seeding aimed at precipitation enhancement are discussed.     

A closure study of sub-micrometer aerosol particle hygroscopic behaviour

The hygroscopic properties of sub-micrometer aerosol particles were studied in connection with a ground-based cloud experiment at Great Dun Fell, in northern England in 1995. Hygroscopic diameter growth factors were measured with a Tandem Differential Mobility Analyser (TDMA) for dry particle diameters between 35 and 265 nm at one of the sites upwind of the orographic cloud. An external mixture consisting of three groups of particles, each with different hygroscopic properties, was observed. These particle groups were denoted less-hygroscopic, more-hygroscopic and sea spray particles and had average diameter growth factors of 1.11–1.15, 1.38–1.69 and 2.08–2.21 respectively when taken from a dry state to a relative humidity of 90%. Average growth factors increased with dry particle size. A bimodal hygroscopic behaviour was observed for 74–87% of the cases depending on particle size. Parallel measurements of dry sub-micrometer particle number size distributions were performed with a Differential Mobility Particle Sizer (DMPS). The inorganic ion aerosol composition was determined by means of ion chromatography analysis of samples collected with Berner-type low pressure cascade impactors at ambient conditions. The number of ions collected on each impactor stage was predicted from the size distribution and hygroscopic growth data by means of a model of hygroscopic behaviour assuming that only the inorganic substances interacted with the ambient water vapour. The predicted ion number concentration was compared with the actual number of all positive and negative ions collected on the various impactor stages. For the impactor stage which collected particles with aerodynamic diameters between 0.17–0.53 μm at ambient relative humidity, and for which all pertinent data was available for the hygroscopic closure study, the predicted ion concentrations agreed with the measured values within the combined measurement and model uncertainties for all cases but one. For this impactor sampling occasion, the predicted ion concentration was significantly higher than the measured. The air mass in which this sample was taken had undergone extensive photochemical activity which had probably produced hygroscopically active material other than inorganic ions, such as organic oxygenated substances.     

Recent Progress of Aerosol Light-scattering Enhancement Factor Studies in China

Assessment of the radiative forcing of aerosols in models still lacks sufficient input data for aerosol hygroscopicity. The light scattering enhancement factor [ f(RH, λ)] is a crucial parameter for describing aerosol hygroscopic growth properties.In this paper, we provide a survey of f(RH, λ) studies in China for the past seven years, including instrument developments of humidified nephelometers, ambient f(RH, λ) measurements in China, f(RH, λ) parameterization schemes, and f(RH, λ)applications in aerosol measurements. Comparisons of different f(RH, λ) parameterizations are carried out to check their performance in China using field measurement datasets. We also summary the parameterization schemes for predicting f(RH, λ)with aerosol chemical compositions. The recently developed methods to observe other aerosol properties using f(RH, λ)measurements, such as calculating the aerosol hygroscopicity parameter, cloud condensation nuclei number concentration,aerosol liquid water content, and aerosol asymmetry factor, are introduced. Suggestions for further research on f(RH, λ) in China are given.     

基于航测的云底气溶胶活化率与过饱和度估算

2016年11月13日在北京地区上空存在持续稳定的层状云天气背景下,利用飞机开展气溶胶粒径谱、化学组成、云滴谱等参量的垂直观测,研究该个例云底气溶胶的活化能力。结果表明:探测期间北京地区为轻度污染天气,地面气溶胶浓度(0.11~3 μm)达到4600 cm-3。云层高度为800~1200 m,云底气溶胶数浓度相对于近地面大幅度降低,有效粒径显著增大(0.3~0.6 μm)。同时,近地面气溶胶中疏水性的一次有机气溶胶贡献显著,而云底气溶胶中一次有机气溶胶的贡献大幅降低,无机组分和二次有机气溶胶的贡献明显增大,造成吸湿性参数κ由0.25(地面)增大至0.32(云底)。云中气溶胶和云滴的谱分布衔接较好,且两者的数浓度之和与云底气溶胶浓度一致,可分别代表未活化和已活化的粒子。基于云底气溶胶粒径谱和吸湿性参数计算得到不同过饱和比下云凝结核的活化率,通过与云中观测结果对比,反推得到云底过饱和度约为0.048%。     

A multifunctional HTDMA system with a robust temperature control

The hygroscopicity of atmospheric aerosols significantly influences their size distribution, cloud condensation nuclei ability, atmospheric residence time, and climate forcing. In order to investigate the hygroscopic behavior of aerosol particles and serious haze in China, a Hygroscopic Tandem Differential Mobility Analyzers (HTDMA) system was designed and constructed at Fudan University. It can function as a scanning mobility particle sizing system to measure particle size distribution in the range of 20--1000 nm in diameter, as well as a hygroscopicity analyzer for aerosol particles with diameters between 20--400 nm in the range of 20%--90% RH (relative humidity). It can also measure the effect of uptake of inorganic acids or semi-VOCs on the hygroscopic behavior of aerosols, such as typical inorganic salts in atmospheric dust or their mixtures. The performance tests show that the system measured particle size of the standard polystyrene latex spheres (PSLs) is 197 nm, which is in excellent agreement with the certified diameter D=199±6 nm, as well as a standard deviation of the repeated runs SD=8.9x10^-4. In addition, the measured hygroscopic growth factors of the model compounds, (NH₄)₂SO₄ and NaNO₃, agree with the Kohler theoretical curves. The results indicate that the HTDMA system is an excellent and powerful tool for studying the hygroscopic behavior of submicron aerosols and meets the demand required for laboratory research and fieldwork on atmospheric aerosols in China.     

State of mixing, shape factor, number size distribution, and hygroscopic growth of the Saharan anthropogenic and mineral dust aerosol at Tinfou, Morocco

The Saharan Mineral Dust Experiment (SAMUM) was conducted in May and June 2006 in Tinfou, Morocco. A H-TDMA system and a H-DMA-APS system were used to obtain hygroscopic properties of mineral dust particles at 85% RH. Dynamic shape factors of 1.11, 1.19 and 1.25 were determined for the volume equivalent diameters 720, 840 and 960 nm, respectively.
During a dust event, the hydrophobic number fraction of 250 and 350 nm particles increased significantly from 30 and 65% to 53 and 75%, respectively, indicating that mineral dust particles can be as small as 200 nm in diameter. Log-normal functions for mineral dust number size distributions were obtained from total particle number size distributions and fractions of hydrophobic particles. The geometric mean diameter for Saharan dust particles was 715 nm during the dust event and 570 nm for the Saharan background aerosol.
Measurements of hygroscopic growth showed that the Saharan aerosol consists of an anthropogenic fraction (predominantly non natural sulphate and carbonaceous particles) and of mineral dust particles. Hygroscopic growth and hysteresis curve measurements of the 'more' hygroscopic particle fraction indicated ammonium sulphate as a main component of the anthropogenic aerosol. Particles larger than 720 nm in diameter were completely hydrophobic meaning that mineral dust particles are not hygroscopic.     

The Great Dun Fell Experiment 1995: an overview

During March and April of 1995 a major international field project was conducted at the UMIST field station site on Great Dun Fell in Cumbria, Northern England. The hill cap cloud which frequently envelopes this site was used as a natural flow through reactor to examine the sensitivity of the cloud microphysics to the aerosol entering the cloud and also to investigate the effects of the cloud in changing the aerosol size distribution, chemical composition and associated optical properties. To investigate these processes, detailed measurements of the cloud water chemistry (including the chemistry of sulphur compounds, organic and inorganic oxidised nitrogen and ammonia), cloud microphysics and properties of the aerosol and trace gas concentrations upwind and downwind of the cap cloud were undertaken. It was found that the cloud droplet number was generally strongly correlated to aerosol number concentration, with up to 2000 activated droplets cm⁻³ being observed in the most polluted conditions. In such conditions it was inferred that hygroscopic organic compounds were important in the activation process. Often, the size distribution of the aerosol was substantially modified by the cloud processing, largely due to the aqueous phase oxidation of S(IV) to sulphate by hydrogen peroxide, but also through the uptake and fixing of gas phase nitric acid as nitrate, increasing the calculated optical scattering of the aerosol substantially (by up to 24%). New particle formation was also observed in the ultrafine aerosol mode (at about 5 nm) downwind of the cap cloud, particularly in conditions of low total aerosol surface area and in the presence of ammonia and HCl gases. This was seen to occur at night as well as during the day via a mechanism which is not yet understood. The implications of these results for parameterising aerosol growth in Global Climate Models are explored.     

Microphysical and chemical characteristics of cloud droplet residuals and interstitial particles in continental stratocumulus clouds

During June and July 2003 the Sources and Origins of Atmospheric Cloud Droplets experiment (SOACED) was carried out on a mountain-top site in central Sweden. The main objective of the experiment was to characterise the microphysical and chemical properties of cloud droplet residuals and interstitial aerosol particles in continental clouds and to understand the processes controlling cloud properties at this location.Interstitial and residual aerosol size distributions, cloud liquid water content and species- and size-resolved aerosol mass concentrations are the main variables employed to address questions pertaining to the cloud droplet number concentration and scavenging efficiency during a stratocumulus cloud event observed on July 28, 2003. In this cloud event, about 56% of the aerosol mass was associated with organic species, whilst SO₄ accounted for 23% and NH₄ for 14%. NO₃ and Cl made up about 7% of the total mass.The partitioning of the aerosol particles between cloud droplets and interstitial air has been studied in terms of their microphysical properties. The scavenging efficiency, defined as the fraction of particles activated into cloud elements compared to the total amount of particles, was investigated as a function of size. The scavenging efficiency curves displayed different shapes during the cloud event, from an S-shaped curve, with low scavenging efficiency in the Aitken mode and larger scavenging efficiency in the accumulation mode, to more unusual shapes where Aitken-mode particles were either solely activated or activated in addition to accumulation-mode particles.This study suggests that alterations of the aerosol chemical composition occurred during the measurement period, changing the hygroscopic nature of the CCN and decreasing their activation diameter. It is also hypothesized that entrainment of drier air aloft may have introduced inhomogeneities in the supersaturation field and modified the S-shaped scavenging curves.     

Microphysical and chemical characteristics of cloud droplet residuals and interstitial particles in continental stratocumulus clouds

During June and July 2003 the Sources and Origins of Atmospheric Cloud Droplets experiment (SOACED) was carried out on a mountain-top site in central Sweden. The main objective of the experiment was to characterise the microphysical and chemical properties of cloud droplet residuals and interstitial aerosol particles in continental clouds and to understand the processes controlling cloud properties at this location.Interstitial and residual aerosol size distributions, cloud liquid water content and species- and size-resolved aerosol mass concentrations are the main variables employed to address questions pertaining to the cloud droplet number concentration and scavenging efficiency during a stratocumulus cloud event observed on July 28, 2003. In this cloud event, about 56% of the aerosol mass was associated with organic species, whilst SO₄ accounted for 23% and NH₄ for 14%. NO₃ and Cl made up about 7% of the total mass.The partitioning of the aerosol particles between cloud droplets and interstitial air has been studied in terms of their microphysical properties. The scavenging efficiency, defined as the fraction of particles activated into cloud elements compared to the total amount of particles, was investigated as a function of size. The scavenging efficiency curves displayed different shapes during the cloud event, from an S-shaped curve, with low scavenging efficiency in the Aitken mode and larger scavenging efficiency in the accumulation mode, to more unusual shapes where Aitken-mode particles were either solely activated or activated in addition to accumulation-mode particles.This study suggests that alterations of the aerosol chemical composition occurred during the measurement period, changing the hygroscopic nature of the CCN and decreasing their activation diameter. It is also hypothesized that entrainment of drier air aloft may have introduced inhomogeneities in the supersaturation field and modified the S-shaped scavenging curves.     

Cloud condensation nuclei spectra derived from size distributions and hygroscopic properties of the aerosol in coastal south-west Portugal during ACE-2

In this work we propose and test a method to calculate cloud condensation nuclei (CCN) spectra based on aerosol number size distributions and hygroscopic growth factors. Sensitivity studies show that this method can be used in a wide variety of conditions except when the aerosol consist mainly of organic compounds. One crucial step in the calculations, estimating soluble ions in an aerosol particle based on hygroscopic growth factors, is tested in an internal hygroscopic consistency study. The results show that during the second Aerosol Characterization Experiment (ACE-2) the number concentration of inorganic ions analyzed in impactor samples could be reproduced from measured growth factors within the measurement uncertainties at the measurement site in Sagres, Portugal.
CCN spectra were calculated based on data from the ACE-2 field experiment at the Sagres site. The calculations overestimate measured CCN spectra on average by approximately 30%, which is comparable to the uncertainties in measurements and calculations at supersaturations below 0.5%. The calculated CCN spectra were averaged over time periods when Sagres received clean air masses and air masses influenced by aged and recent pollution. Pollution outbreaks enhance the CCN concentrations at supersaturations near 0.2% by a factor of 3 (aged pollution) to 5 (recent pollution) compared to the clean marine background concentrations. In polluted air masses, the shape of the CCN spectra changes. The clean spectra can be approximated by a power function, whereas the polluted spectra are better approximated by an error function.     

Hygroscopicity of pre-existing particle distribution and formation of cloud droplets: a model study

The effects of the hygroscopicity of a pre-existing particle distribution and condensation of nitric acid on cloud droplet formation were studied by using an air parcel and multicomponent condensation model. The pre-existing particle distribution used is a bimodal distribution in which the particles are assumed to be internally mixed, i.e. they are composed partly from ammonium nitrate salt and partly from some insoluble substance. The mean diameters of the distributions and the mass fraction of soluble salt were varied in the simulations. Generally, the number of activated cloud droplets was found to be increased, when the initial mass fraction of salt (i.e. the initial amount of salt) was increased. However, the effects of increased initial amount of salt on the cloud droplet formation were not straightforward in all cases studied. The effects of the condensing hygroscopic substance, with initial nitric acid concentrations of 0.1, 1.0 and 10.0 ppbv on the activation of cloud droplets were also studied. The number of activated droplets increased when the initial concentration of nitric acid was increased.     

The effect of clouds on aerosol growth in the rural atmosphere

Measurements of accumulation mode aerosol in the atmospheric boundary layer under cloudy and cloud-free conditions, and in the lower free troposphere under cloud-free conditions, were conducted over the rural northwest of England. Normalised size distributions in the cloud-free boundary layer (CFBL) and the cloud-free free troposphere (CFFT) exhibited almost identical spectral similarities with both size distributions possessing a concentration peak mode-radius of ≈0.05 μm or less. By comparison, aerosol distributions observed in cloudy air exhibited a distinctive log-normal distribution with mode-radii occurring at ≈0.1 μm concomitant with a local minimum at ≈0.05 μm. The consistent and noticeable difference in spectral features observed between cloudy and cloud-free conditions suggest that a greater amount of gas-to-particle conversion occurs on cloudy days, presumably through in-cloud aqueous phase oxidation processes, leading to larger sized accumulation mode particles. Apart from the distinct difference between cloudy and cloud-free aerosol spectra on cloudy days, aerosol concentration and mass were observed to be significantly enhanced above that of the ambient background in the vicinity of clouds. Volatility analysis during one case of cloud processing indicated an increase in the relative contribution of aerosol mass volatile at temperatures characteristic of sulphuric acid, along with a smaller fraction of more volatile material (possibly nitric acid and/or organic aerosol). Growth-law analysis of possible growth mechanisms point to aqueous phase oxidation of aerosol precursors in cloud droplets as being the only feasible mechanism capable of producing the observed growth. The effect of cloud processing is to alter the cloud condensation nuclei (CCN) supersaturation spectrum in a manner which increases the availability of CCN at lower cloud supersaturations.     

Aerosol Hygroscopicity during the Haze Red-Alert Period in December 2016 at a Rural Site of the North China Plain

A humidification system was deployed to measure aerosol hygroscopicity at a rural site of the North China Plain during the haze red-alert period 17–22 December 2016. The aerosol scattering coefficients under dry [relative humidity (RH) < 30%] and wet (RH in the range of 40%–85%) conditions were simultaneously measured at wavelengths of 450, 550, and 700 nm. It is found that the aerosol scattering coefficient and backscattering coefficient increased by only 29% and 10%, respectively when RH went up from 40% to 80%, while the hemispheric backscatter fraction went down by 14%, implying that the aerosol hygroscopicity represented by the aerosol scattering enhancement factor f(RH) is relatively low and RH exerted little effects on the aerosol light scattering in this case. The scattering enhancement factors do not show significant differences at the three wavelengths, only with an approximate 2% variation, suggesting that the aerosol hygroscopicity is independent of the wavelength. Aerosol hygroscopicity is highly dependent on the aerosol chemical composition. When there is a large mass fraction of inorganics and a small mass fraction of organic matter, f(RH) reaches a high value. The fraction of NO₃^– was strongly correlated with the aerosol scattering coefficient at RH = 80%, which suggests that NO₃^– played an important role in aerosol hygroscopic growth during the heavy pollution period.     

On the use of a modified clean-room optical particle counter for atmosperic aerosols at high relative humidity

This study is devoted to the performance of the CLIMET CI-8060, a white-light optical particle counter (OPC). Designed for clean-room monitoring, the off-the-shelf performance of this instrument is rather poor for outdoor studies. Modifications of this instrument are described turning this low-cost instrument into an OPC with excellent performance. The modifications include a reduction of the flow rate to 1.4 l/min, an altered design of the inlet nozzle, a buffer chamber to assure continuous flow, and a 16-channel pulse height analyzer.The modified version has been checked thouroughly. The counting efficiency is very close to 100% for particle sizes between 0.295 and 0.801 μm. The loss of giant particles is also marginal, as comparative tests with a cascade impactor show. The sizing calibration has been redetermined experimentally, using latex spheres, and theoretically, applying a software package by Jüngert [1988] using the Mie theory. With the help of the established relationship between experimental and theoretical response for latex, calibration tables for any other particle material are obtained (in particular for ambient aerosols and H₂O for fog and cloud condensation studies).The modified counter has been used for monitoring the growth of hygroscopic aerosols in humid conditions, using two different inlet lines, one of them drying the aerosol before entering the OPC, the other one preserving ambient conditions. This system allows to observe haze and fog formation and cloud condensation processes in situ at a one-minute time resolution.     

黄山地区气溶胶吸湿增长特性数值模拟研究

应用多种化学组分气溶胶的绝热气块分档模式,对2008年春季黄山地区气溶胶吸湿增长特性进行了模拟分析.结果表明:黄山地区气溶胶吸湿增长因子f的大小与粒子半径、相对湿度、粒子化学组分、上升速度及上升高度密切相关,且小粒子吸湿增长比大粒子显著.吸湿增长因子与相对湿度呈正相关,相对湿度越接近粒子的临界饱和比,吸湿增长因子变化越显著.可溶性有机气溶胶,通过增加溶液中溶质的百分比来影响临界饱和比,使吸湿增长因子增大.若不考虑不可溶粒子的成核作用,会高估粒子的吸湿性.随着上升速度增大,吸湿增长因子降低,降低程度与粒子初始高度的相对湿度有关.上升高度通过改变气块相对湿度的变化来影响气溶胶吸湿增长因子.     

Kinetic limitations on cloud droplet formation and impact on cloud albedo

Under certain conditions mass transfer limitations on the growth of cloud condensation nuclei (CCN) may have a significant impact on the number of droplets that can form in a cloud. The assumption that particles remain in equilibrium until activated may therefore not always be appropriate for aerosol populations existing in the atmosphere. This work identifies three mechanisms that lead to kinetic limitations, the effect of which on activated cloud droplet number and cloud albedo is assessed using a one‐dimensional cloud parcel model with detailed microphysics for a variety of aerosol size distributions and updraft velocities. In assessing the effect of kinetic limitations, we have assumed as cloud droplets not only those that are strictly activated (as dictated by classical Köhler theory), but also unactivated drops large enough to have an impact on cloud optical properties. Aerosol number concentration is found to be the key parameter that controls the significance of kinetic effects. Simulations indicate that the equilibrium assumption leads to an overprediction of droplet number by less than 10% for marine aerosol; this overprediction can exceed 40% for urban type aerosol. Overall, the effect of kinetic limitations on cloud albedo can be considered important when equilibrium activation theory consistently overpredicts droplet number by more than 10%. The maximum change in cloud albedo as a result of kinetic limitations is less than 0.005 for cases such as marine aerosol; however albedo differences can exceed 0.1 under more polluted conditions. Kinetic limitations are thus not expected to be climatically significant on a global scale, but can regionally have a large impact on cloud albedo.     

The chemical fractionation of atmospheric aerosol as a result of snow crystal formation and growth

The relationships between the physical and chemical properties of mixed-phase clouds were investigated at Storm Peak Laboratory (3220m MSL) located near the continental divide in northwestern Colorado. Interstitial aerosol particles, cloud droplets and snow crystals were concurrently collected when the laboratory was enveloped by a precipitating cloud. All samples were analyzed for trace elements, soluble anions, electrical conductivity and acidity.The results show average trace constituent concentration ratios of cloud water to snow water range from 0.4 to 26. All but six of the 32 elements and ions measured had ratios greater than one. This result suggests a chemical species dependency of in-cloud aerosol particle scavenging processes. Evidence of a decrease of in-cloud aerosol particle scavenging efficiency by snow due to increases in aerosol concentration is also presented.Differences between the chemical composition of cloud water and snow water are manifested most strongly when snow crystals grow by vapor deposition. In-cloud scavenging efficiencies by snow crystals for most aerosol particle chemical species are dependent on the growth of the snow crystals by accretion of cloud droplets. This chemical fractionation of the atmospheric aerosol by snow crystal formation and growth should be most active where narrow, continental cloud droplet size distributions and low liquid water contents are prevalent, enhancing the probability of snow crystal growth by diffusion.