Inland sources of particulate chloride for atmospheric nitryl chloride (ClNO 2 ) formation remain unknown and unquantified, hindering air quality assessments. Globally each winter, tens of millions of tons of road salt are spread on roadways for deicing. Here, we identify road salt aerosol as the primary chloride aerosol source, accounting for 80−100% of ClNO 2 formation, at an inland urban area in the wintertime. This study provides experimental evidence of the connection between road salt and air quality through the production of this important reservoir for nitrogen oxides and chlorine radicals, which significantly impact atmospheric composition and pollutant fates. A numerical model was employed to quantify the contributions of chloride sources to ClNO 2 production. The traditional method for simulating ClNO 2 considers chloride to be homogeneously distributed across the atmospheric particle population; yet, we show that only a fraction of the particulate surface area contains chloride. Our new single-particle parametrization considers this heterogeneity, dramatically lowering overestimations of ClNO 2 levels that have been routinely reported using the prevailing methods. The identification of road salt as a ClNO 2 source links this common deicing practice to atmospheric composition and air quality in the urban wintertime environment.

Abstract. Aerosols that serve as ice nucleating particles (INPs) have the potential to modulate cloud microphysical properties and can therefore impact cloud radiative forcing (CRF) and precipitation formation processes. In remote regions such as the Arctic, aerosol–cloud interactions are severely understudied yet may have significant implications for the surface energy budget and its impact on sea ice and snow surfaces. Further, uncertainties in model representations of heterogeneous ice nucleation are a significant hindrance to simulating Arctic mixed-phase cloud processes. We present results from a campaign called INPOP (Ice Nucleating Particles at Oliktok Point), which took place at a US Department of Energy Atmospheric Radiation Measurement (DOE ARM) facility in the northern Alaskan Arctic. Three time- and size-resolved aerosol impactors were deployed from 1 March to 31 May 2017 for offline ice nucleation and chemical analyses and were co-located with routine measurements of aerosol number and size. The largest particles (i.e., ≥ 3 µm or “coarse mode”) were the most efficient INPs by inducing freezing at the warmest temperatures. During periods with snow- and ice-covered surfaces, coarse mode INP concentrations were very low (maximum of 6 × 10−4 L−1 at −15 ∘C), but higher concentrations of warm-temperature INPs were observed during late May (maximum of 2 × 10−2 L−1 at −15 ∘C). These higher concentrations were attributed to air masses originating from over open Arctic Ocean water and tundra surfaces. To our knowledge, these results represent the first INP characterization measurements in an Arctic oilfield location and demonstrate strong influences from mineral and marine sources despite the relatively high springtime pollution levels. Ultimately, these results can be used to evaluate the anthropogenic and natural influences on aerosol composition and Arctic cloud properties.

The Arctic is experiencing the greatest warming on Earth, as most evident by rapid sea ice loss. Delayed sea ice freeze-up in the Alaskan Arctic is decreasing wintertime sea ice extent and changing marine biological activity. However, the impacts of newly open water on wintertime sea spray aerosol (SSA) production and atmospheric composition are unknown. Herein, we identify SSA, produced locally from open sea ice fractures (leads), as the dominant aerosol source in the coastal Alaskan Arctic during winter, highlighting the year-round nature of Arctic SSA emissions. Nearly all of the individual SSA featured thick organic coatings, consisting of marine saccharides, amino acids, fatty acids, and divalent cations, consistent with exopolymeric secretions produced as cryoprotectants by sea ice algae and bacteria. In contrast, local summertime SSA lacked these organic carbon coatings, or featured thin coatings, with only open water nearby. The individual SSA composition was not consistent with frost flowers or surface snow above sea ice, suggesting that neither hypothesized frost flower aerosolization nor blowing snow sublimation resulted in the observed SSA. These results further demonstrate the need for inclusion of lead-based SSA production in modeling of Arctic atmospheric composition. The identified connections between changing sea ice, microbiology, and SSA point to the significance of sea ice lead biogeochemistry in altering Arctic atmospheric composition, clouds, and climate feedbacks during winter.

In freshwater lakes, harmful algal blooms (HABs) of Cyanobacteria (blue-green algae) produce toxins that impact human health. However, little is known about the lake spray aerosol (LSA) produced from wave-breaking in freshwater HABs. In this study, LSA were produced in the laboratory from freshwater samples collected from Lake Michigan and Lake Erie during HAB and nonbloom conditions. The incorporation of biological material within the individual HAB-influenced LSA particles was examined by single-particle mass spectrometry, scanning electron microscopy with energy-dispersive X-ray spectroscopy, and fluorescence microscopy. Freshwater with higher blue-green algae content produced higher number fractions of individual LSA particles that contained biological material, showing that organic molecules of biological origin are incorporated in LSA from HABs. The number fraction of individual LSA particles containing biological material also increased with particle diameter (greater than 0.5 μm), a size dependence that is consistent with previous studies of sea spray aerosol impacted by phytoplankton blooms. Similar to sea spray aerosol, organic carbon markers were most frequently observed in individual LSA particles less than 0.5 μm in diameter. Understanding the transfer of biological material from freshwater to the atmosphere via LSA is crucial for determining health and climate effects of HABs.