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Modeling of atmosphere–snow exchange provides insight into fundamental processes driving pollutant deposition. Gas properties, such as solubility and stickiness to ice, influence the role of the snowpack as a trace gas reservoir and chemical reactor. 

The Alaskan Layered Pollution And Chemical Analysis (ALPACA)-2022 field study (https://alpaca.community.uaf.edu/alpaca-field-study/) investigated air pollution under dark and cold conditions in Fairbanks, Alaska in January and February, 2022. One of the main motivations for ALPACA was to understand how temperature inversions trap pollutants at the surface. This was studied by using University of California, Los Angeles (UCLA) long-path Differential Optical Absorption Spectroscopy instrument (LP-DOAS) to probe the Fairbanks atmosphere from 12 meters(m) – 191m altitude and yield information on the vertical distribution of various trace gases / pollutants. The dataset contains the open atmosphere LP-DOAS measurement of Ozone (O3), Sulfur Dioxide (SO2), Nitrogen Dioxide (NO2), Formaldehyde (HCHO), and Nitrous Acid (HONO) on four different light paths over wintertime downtown Fairbanks, Alaska (AK) during ALPACA. The four light paths cover the following altitude intervals: 12-17m, 17-73m, 17-115m, and 17-191m. The ReadMe file included in the data set provides exact coordinates, length, and altitude intervals for the four light paths. 

Abstract. Subarctic cities notoriously experience severe winter pollution episodes with fine particle (PM2.5) concentrations above 35 µg m−3, the US Environmental Protection Agency (EPA) 24 h standard. While winter sources of primary particles in Fairbanks, Alaska, have been studied, the chemistry driving secondary particle formation is elusive. Biomass burning is a major source of wintertime primary particles, making the PM2.5 rich in light-absorbing brown carbon (BrC). When BrC absorbs sunlight, it produces photooxidants – reactive species potentially important for secondary sulfate and secondary organic aerosol formation – yet photooxidant measurements in high-latitude PM2.5 remain scarce. During the winter of 2022 Alaskan Layered Pollution And Chemical Analysis (ALPACA) field campaign in Fairbanks, we collected PM filters, extracted the filters into water, and exposed the extracts to simulated sunlight to characterize the production of three photooxidants: oxidizing triplet excited states of BrC, singlet molecular oxygen, and hydroxyl radical. Next, we used our measurements to model photooxidant production in highly concentrated aerosol liquid water. While conventional wisdom indicates photochemistry is limited during high-latitude winters, we find that BrC photochemistry is significant: we predict high triplet and singlet oxygen daytime particle concentrations up to 2×10-12 and 3×10-11 M, respectively, with moderate hydroxyl radical concentrations up to 5×10-15 M. Although our modeling predicts that triplets account for 0.4 %–10 % of daytime secondary sulfate formation, particle photochemistry cumulatively dominates, generating 76 % of daytime secondary sulfate formation, largely due to in-particle hydrogen peroxide, which contributes 25 %–54 %. Finally, we estimate triplet production rates year-round, revealing the highest rates in late winter when Fairbanks experiences severe pollution and in summer when wildfires generate BrC. 

Fairbanks-North Star Borough, Alaska (FNSB) regularly experiences some of the worst wintertime air quality in the United States. 

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. 

Fairbanks-North Star Borough (FNSB), Alaska perennially experiences some of the worst wintertime air quality in the United States. FNSB was designated as a “serious” nonattainment area by the U.S. Environmental Protection Agency in 2017 for excessive fine particulate matter (PM 2.5 ) concentrations. The ALPACA (Alaskan Layered Pollution And Chemical Analysis) field campaign was established to understand the sources of air pollution, pollutant transformations, and the meteorological conditions contributing to FNSB's air quality problem. We performed on-road mobile sampling during ALPACA to identify and understand the spatial patterns of PM across the study domain, which contained multiple stationary field sites and regulatory measurement sites. Our measurements demonstrate the following: (1) both the between-neighborhood and within-neighborhood variations in PM 2.5 concentrations and composition are large (>10 μg m −3 ). (2) Spatial variations of PM in Fairbanks are tightly connected to meteorological conditions; dramatic between-neighborhood differences exist during strong temperature inversion conditions, but are significantly reduced during weaker temperature inversions, where atmospheric conditions are more well mixed. (3) During strong inversion conditions, total PM 2.5 and black carbon (BC) are tightly spatially correlated and have high absorption Ångstrom exponent values (AAE > 1.4), but are relatively uncorrelated during weak inversion conditions and have lower AAE. (4) PM 2.5 , BC, and total particle number (PN) concentrations decreased with increasing elevation, with the fall-off being more dramatic during strong temperature inversion conditions. (5) Mobile sampling reveals important air pollutant concentration differences between the multiple fixed sites of the ALPACA study, and demonstrates the utility of adding mobile sampling for understanding the spatial context of large urban air quality field campaigns. These results are important for understanding both the PM exposure for residents of FNSB and the spatial context of the ALPACA study. 

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.