气候变化领域集成服务门户(CCPortal): Atmospheric biogenic volatile organic compounds in the Alaskan Arctic tundra: constraints from measurements at Toolik Field Station

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DOI	10.5194/acp-22-14037-2022
	Atmospheric biogenic volatile organic compounds in the Alaskan Arctic tundra: constraints from measurements at Toolik Field Station
	Selimovic, Vanessa; Ketcherside, Damien; Chaliyakunnel, Sreelekha; Wielgasz, Catherine; Permar, Wade; Angot, Helene; Millet, Dylan B.; Fried, Alan; Helmig, Detlev; Hu, Lu
发表日期	2022
ISSN	1680-7316
EISSN	1680-7324
起始页码	14037
结束页码	14058
卷号	22 期号:21 页码:22
英文摘要	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 degrees 38' N, 149 degrees 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 degrees x 0.3125 degrees 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 exponentially with air temperature, likely reflecting its biogenic precursors and pointing to a systematic model underprediction of its secondary production. The median campaign-calculated OHr from VOCs measured at TFS was 0.7 s(-1), roughly 5 % of the values typically reported in lower-latitude forested ecosystems. Ten species account for over 80 % of the calculated VOC OHr, with formaldehyde, isoprene and acetaldehyde together accounting for nearly half of the total. Simulated OHr based on median-modeled VOCs included in GEOS-Chem averages 0.5 s(-1) and is dominated by isoprene (30 %) and monoterpenes (17 %). The data presented here serve as a critical evaluation of our knowledge of BVOCs and ROC budgets in high-latitude environments and represent a foundation for investigating and interpreting future warming-driven changes in VOC emissions in the Alaskan Arctic tundra.
学科领域	Environmental Sciences; Meteorology & Atmospheric Sciences
语种	英语
WOS研究方向	Environmental Sciences & Ecology ; Meteorology & Atmospheric Sciences
WOS记录号	WOS:000877651100001
来源期刊	ATMOSPHERIC CHEMISTRY AND PHYSICS
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/273066
作者单位	University of Montana System; University of Montana; University of Colorado System; University of Colorado Boulder; University of Minnesota System; University of Minnesota Twin Cities; Swiss Federal Institutes of Technology Domain; Ecole Polytechnique Federale de Lausanne
推荐引用方式 GB/T 7714	Selimovic, Vanessa,Ketcherside, Damien,Chaliyakunnel, Sreelekha,et al. Atmospheric biogenic volatile organic compounds in the Alaskan Arctic tundra: constraints from measurements at Toolik Field Station[J],2022,22(21):22.
APA	Selimovic, Vanessa.,Ketcherside, Damien.,Chaliyakunnel, Sreelekha.,Wielgasz, Catherine.,Permar, Wade.,...&Hu, Lu.(2022).Atmospheric biogenic volatile organic compounds in the Alaskan Arctic tundra: constraints from measurements at Toolik Field Station.ATMOSPHERIC CHEMISTRY AND PHYSICS,22(21),22.
MLA	Selimovic, Vanessa,et al."Atmospheric biogenic volatile organic compounds in the Alaskan Arctic tundra: constraints from measurements at Toolik Field Station".ATMOSPHERIC CHEMISTRY AND PHYSICS 22.21(2022):22.