Atmospheric biogenic volatile organic compounds in the Alaskan Arctic tundra: constraints from measurements at Toolik Field Station

• Published in: Atmospheric Chemistry and Physics
• Main Authors: V. Selimovic, D. Ketcherside, S. Chaliyakunnel, C. Wielgasz, W. Permar, H. Angot, D. B. Millet, A. Fried, D. Helmig, L. Hu
• Format: Article in Journal/Newspaper
• Language: English
• Published: Copernicus Publications 2022
• Subjects: Physics; QC1-999; Chemistry; QD1-999; Arctic; Tundra; Alaska
• Online Access: https://doi.org/10.5194/acp-22-14037-2022; https://doaj.org/article/0ee1da8cb9ee408d86dd2f69fd421f0c

The Arctic is a climatically sensitive region that has experienced warming at almost 3 times the global average rate in recent decades, leading to an increase in Arctic greenness and a greater abundance of plants that emit biogenic volatile organic compounds (BVOCs). These changes in atmospheric emissions are expected to significantly modify the overall oxidative chemistry of the region and lead to changes in VOC composition and abundance, with implications for atmospheric processes. Nonetheless, observations needed to constrain our current understanding of these issues in this critical environment are sparse. This work presents novel atmospheric in situ proton-transfer-reaction time-of-flight mass spectrometry (PTR-ToF-MS) measurements of VOCs at Toolik Field Station (TFS; 68 ∘ 38 ′ N, 149 ∘ 36' W), in the Alaskan Arctic tundra during May–June 2019. We employ a custom nested grid version of the GEOS-Chem chemical transport model (CTM), driven with MEGANv2.1 (Model of Emissions of Gases and Aerosols from Nature version 2.1) biogenic emissions for Alaska at 0.25 ∘ × 0.3125 ∘ resolution, to interpret the observations in terms of their constraints on BVOC emissions, total reactive organic carbon (ROC) composition, and calculated OH reactivity (OHr) in this environment. We find total ambient mole fraction of 78 identified VOCs to be 6.3 ± 0.4 ppbv (10.8 ± 0.5 ppbC), with overwhelming ( > 80 %) contributions are from short-chain oxygenated VOCs (OVOCs) including methanol, acetone and formaldehyde. Isoprene was the most abundant terpene identified. GEOS-Chem captures the observed isoprene (and its oxidation products), acetone and acetaldehyde abundances within the combined model and observation uncertainties ( ±25 %), but underestimates other OVOCs including methanol, formaldehyde, formic acid and acetic acid by a factor of 3 to 12. The negative model bias for methanol is attributed to underestimated biogenic methanol emissions for the Alaskan tundra in MEGANv2.1. Observed formaldehyde mole fractions increase ...