Physicochemical processes of nucleation constitute a major uncertainty in understanding aerosol‐cloud interactions. To improve the knowledge of the ice nucleation process, we characterized physical, chemical, and biological properties of fresh snow using a suite of state‐of‐the‐art techniques based on mass spectrometry, electron microscopy, chromatography, and optical particle sizing. Samples were collected at two North American Arctic sites, as part of international campaigns (2006 and 2009), and in the city of Montreal, Canada, over the last decade. Particle size distribution analyses, in the range of 3 nm to 10 µm, showed that nanosized particles are the most numerous (38–71%) in fresh snow, with a significant portion (11 to 19%) less than 100 nm in size. Particles with diameters less than 200 nm consistently exhibited relatively high ice‐nucleating properties (on average ranged from −19.6 ± 2.4 to −8.1 ± 2.6°C). Chemical analysis of the nanosized fraction suggests that they contain bioorganic materials, such as amino acids, as well as inorganic compounds with similar characteristics to mineral dust. The implication of nanoparticle ubiquity and abundance in diverse snow ecosystems are discussed in the context of their importance in understanding atmospheric nucleation processes.

Little is known about pollution in urban snow and how aerosol and gaseous air pollutants interact with the urban snowpack. Here we investigate interactions of exhaust pollution with snow at low ambient temperature using fresh snow in a temperature-controlled chamber. A gasoline-powered engine from a modern light duty vehicle generated the exhaust and was operated in homogeneous and stratified engine regimes. We determined that, within a timescale of 30 min, snow takes up from the exhaust a large mass of organic pollutants and aerosol particles, which were observed by electron microscopy, mass spectrometry and aerosol sizers. Specifically, the concentration of total organic carbon in the exposed snow increased from 0.948 ± 0.009 to 1.828 ± 0.001 mg/L (homogeneous engine regime) and from 0.275 ± 0.005 to 0.514 ± 0.008 mg/L (stratified engine regime). The concentrations of benzene, toluene and 13 out of 16 measured polycyclic aromatic hydrocarbons (PAHs), particularly naphthalene, benz[a]anthracene, chrysene and benzo[a]pyrene in snow increased upon exposure from near the detection limit to 0.529 ± 0.058, 1.840 ± 0.200, 0.176 ± 0.020, 0.020 ± 0.005, 0.025 ± 0.005 and 0.028 ± 0.005 ng/kg, respectively, for the homogeneous regime. After contact with snow, 50-400 nm particles were present with higher relative abundance compared to the smaller nanoparticles (<50 nm), for the homogeneous regime. The lowering of temperature from 25 ± 1 °C to (-8) - (-10) ± 1 °C decreased the median mode diameter of the exhaust aerosol particles from 69 nm to 57 nm (p < 0.1) and addition of snow to 51 nm (p < 0.1) for the stratified regime, but increased it from 20 nm to 27 nm (p < 0.1) for the homogeneous regime. Future studies should focus on cycling of exhaust-derived pollutants between the atmosphere and cryosphere. The role of the effects we discovered should be evaluated as part of assessment of pollutant loads and exposures in regions with a defined winter season.

Snowpacks in the Alberta Oil Sands Region (AOSR) of Canada contain elevated loadings of methylmercury (MeHg; a neurotoxin that biomagnifies through foodwebs) due to oil sands related activities. At sites ranging from 0 to 134 km from the major AOSR upgrading facilities, we examined sources of MeHg by quantifying potential rates of MeHg production in snowpacks and melted snow using mercury stable isotope tracer experiments, as well as quantifying concentrations of MeHg on particles in snowpacks (pMeHg). At four sites, methylation rate constants were low in snowpacks (k = 0.001-0.004 d) and nondetectable in melted snow, except at one site (k = 0.0007 d). The ratio of methylation to demethylation varied between 0.3 and 1.5, suggesting that the two processes are in balance and that in situ production is unlikely an important net source of MeHg to AOSR snowpacks. pMeHg concentrations increased linearly with distance from the upgraders (R = 0.71, p < 0.0001); however, snowpack total particle and pMeHg loadings decreased exponentially over this same distance (R = 0.49, p = 0.0002; R = 0.56, p < 0.0001). Thus, at near-field sites, total MeHg loadings in snowpacks were high due to high particle loadings, even though particles originating from industrial activities were not MeHg rich compared to those at remote sites. More research is required to identify the industrial sources of snowpack particles in the AOSR.

Exposure to vehicle exhaust can drive up to 70 % of excess lifetime cancer incidences due to air pollution in urban environments. Little is known about how exhaust-derived particles and organic pollutants, implicated in adverse health effects, are affected by freezing ambient temperatures and the presence of snow. Airborne particles and (semi)volatile organic constituents in dilute exhaust were studied in a novel low-temperature environmental chamber system containing natural urban snow under controlled cold environmental conditions. The presence of snow altered the aerosol size distributions of dilute exhaust in the 10 nm to 10 μm range and decreased the number density of the nanoparticulate (<100 nm) fraction of exhaust aerosols, yet increased the 100-150 nm fraction. Upon 1 hour exhaust exposure, the total organic carbon increased in the natural snow from 0.218 ± 0.014 to 0.539 ± 0.009 mg L(-1), and over 40 additional (semi)volatile organic compounds and a large number of exhaust-derived carbonaceous and likely organic particles were identified. The concentrations of benzene, toluene, ethylbenzene, and xylenes (BTEX) increased from near the detection limit to 52.48, 379.5, 242.7, and 238.1 μg kg(-1) (± 10 %), respectively, indicating the absorption of exhaust-derived toxic organic compounds by snow. The alteration of exhaust aerosol size distributions at freezing temperatures and in the presence of snow, accompanied by changes of the organic pollutant content in snow, has potential to alter health effects of human exposure to vehicle exhaust.

Tropospheric aerosols are involved in several key atmospheric processes: from ice nucleation, cloud formation, and precipitation to weather and climate. The impact of aerosols on these atmospheric processes depends on the chemical and physical characteristics of aerosol particles, and these characteristics are still largely uncertain. In this study, we developed a system for processing and aerosolization of melted snow in particle-free air, coupled with a real-time measurement of aerosol size distributions. The newly developed technique involves bringing snow-borne particles into an airborne state, which enables application of high-resolution aerosol analysis and sampling techniques. This novel analytical approach was compared to a variety of complementary existing analytical methods as applied for characterization of snow samples from remote sites in Alert (Canada) and Barrow (USA), as well as urban Montreal (Canada). The dry aerosol measurements indicated a higher abundance of particles of all sizes, and the 30 nm size dominated in aerosol size distributions for the Montreal samples, closely followed by Barrow, with about 30% fewer 30 nm particles, and about four times lower 30 nm particle abundance in Alert samples, where 15 nm particles were most abundant instead. The aerosolization technique, used together with nanoparticle tracking analysis and electron microscopy, allowed measurement of a wide size range of snow-borne particles in various environmental snow samples. Here, we discuss the application of the new technique to achieve better physicochemical understanding of atmospheric and snow processes. The results showed high sensitivity and reduction of particle aggregation, as well as the ability to measure a high-resolution snow-borne particle size distribution, including nanoparticulate matter in the range of 10 to 100 nm.