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The prevailing view for aqueous secondary aerosol formation is that it occurs in clouds and fogs, owing to the large liquid water content compared to minute levels in fine particles. Our research indicates that this view may need reevaluation due to enhancements in aqueous reactions in highly concentrated small particles. Here, we show that low temperature can play a role through a unique effect on particle pH that can substantially modulate secondary aerosol formation. Marked increases in hydroxymethanesulfonate observed under extreme cold in Fairbanks, Alaska, demonstrate the effect. These findings provide insight on aqueous chemistry in fine particles under cold conditions expanding possible regions of secondary aerosol formation that are pH dependent beyond conditions of high liquid water. 

Abstract. Fairbanks, Alaska, is a sub-Arctic city that frequently suffers from the non-attainment of national air quality standards in the wintertime due to the coincidence of weak atmospheric dispersion and increased local emissions. As part of the Alaskan Layered Pollution and Chemical Analysis (ALPACA) campaign, we deployed a Chemical Analysis of Aerosol Online (CHARON) inlet coupled with a proton transfer reaction time-of-flight mass spectrometer (PTR-ToF MS) and an Aerodyne high-resolution aerosol mass spectrometer (AMS) to measure organic aerosol (OA) and non-refractory submicron particulate matter (NR-PM1), respectively. We deployed a positive matrix factorization (PMF) analysis for the source identification of NR-PM1. The AMS analysis identified three primary factors: biomass burning, hydrocarbon-like, and cooking factors, which together accounted for 28 %, 38 %, and 11 % of the total OA, respectively. Additionally, a combined organic and inorganic PMF analysis revealed two further factors: one enriched in nitrates and another rich in sulfates of organic and inorganic origin. The PTRCHARON factorization could identify four primary sources from residential heating: one from oil combustion and three from wood combustion, categorized as low temperature, softwood, and hardwood. Collectively, all residential heating factors accounted for 79 % of the total OA. Cooking and road transport were also recognized as primary contributors to the overall emission profile provided by PTRCHARON. All PMF analyses could apportion a single oxygenated secondary organic factor. These results demonstrate the complementarity of the two instruments and their ability to describe the complex chemical composition of PM1 and related sources. This work further demonstrates the capability of PTRCHARON to provide both qualitative and quantitative information, offering a comprehensive understanding of the OA sources. Such insights into the sources of submicron aerosols can ultimately assist environmental regulators and citizens in improving the air quality in Fairbanks and in rapidly urbanizing regional sub-Arctic areas. 

Abstract We investigated how various sources contributed to observations of over 40 trace gas and particulate species in a typical Fairbanks residential neighborhood during the Alaskan Layered Pollution and Chemical Analysis campaign in January–February 2022. Aromatic volatile organic compounds (VOCs) accounted for ∼50% of measured VOCs (molar ratio), while methanol and ethanol accounted for ∼34%. The total wintertime VOC burden and contribution from aromatics were much higher than other US urban areas. Based on diel cycles and positive matrix factorization (PMF) analyses, we find traffic was the largest source of NO, CO, black carbon, and aromatic VOCs. Formic and acetic acid, hydroxyacetone, furanoids, and other VOCs were primarily attributed to residential wood combustion (RWC). Formaldehyde was one of several VOCs featuring significant contributions from multiple sources: RWC (∼35%), aging (∼30%), traffic (∼21%), and heating oil combustion (HO, ∼14%). PMF solutions assigned primary fine particulate matter to RWC (10%–30%), traffic (25%–40%), and HO (30%–60%), the latter likely reflecting high sulfur emissions from older furnaces and fast secondary chemistry. Despite cold and dark conditions, secondary processes impacted many trace gas and particle species' budget by ±10%–20% and more in some cases. Transport of O₃‐rich regional air into Fairbanks contributed to aging, specifically NO₃radical formation. This work highlights a long‐term trend observed in Fairbanks: increasing traffic and decreasing RWC relative contributions as total pollution decreases. Fairbanks exports a relatively fresh pollutant mixture to the regional arctic, the fate of which warrants future study. 

Abstract The Alaskan Layered Pollution and Chemical Analysis (ALPACA) field campaign included deployment of a suite of atmospheric measurements in January–February 2022 with the goal of better understanding atmospheric processes and pollution under cold and dark conditions in Fairbanks, Alaska. We report on measurements of particle composition, particle size, ice nucleating particle (INP) composition, and INP size during an ice fog period (29 January–3 February). During this period, coarse particulate matter (PM₁₀) concentrations increased by 150% in association with a decrease in air temperature, a stronger temperature inversion, and relatively stagnant conditions. Results also show a 18%–78% decrease in INPs during the ice fog period, indicating that particles had activated into the ice fog via nucleation. Peroxide and heat treatments performed on INPs indicated that, on average, the largest contributions to the INP population were heat‐labile (potentially biological, 63%), organic (31%), then inorganic (likely dust, 6%). Measurements of levoglucosan and bulk and single‐particle composition corroborate the presence of dust and aerosols from combustion sources. Heat‐labile and organic INPs decreased during the peak period of the ice fog, indicating those were preferentially activated, while inorganic INPs increased, suggesting they remained as interstitial INPs. In general, INP concentrations were unexpectedly high in Fairbanks compared to other locations in the Arctic during winter. The fact that these INPs likely facilitated ice fog formation in Fairbanks has implications for other high latitude locations subject to the hazards associated with ice fog.