Organic Functional Groups in the Submicron Aerosol at 82.5° N from 2012 to 2014

摘要

The first multi-year contributions from organic functional groups to the Arctic submicron aerosol are documented using 126 weekly-integrated samples collected from April, 2012 to October, 2014 at the Alert Observatory (82.45° N, 62.51° W). Results from the particle transport model FLEXPART, linear regressions among the organic and inorganic components and Positive Matrix Factorization (PMF) enable associations of organic aerosol components with source types and regions. Lower organic mass concentrations (OM) but higher ratios of OM to non-sea-salt sulphate mass concentrations (nss-SO) accompany smaller particles during the summer (JJA). Conversely, higher OM but lower OM/nss-SO accompany larger particles during winter-spring. OM ranges from 7–463 ng m, and the study average is 129 ng m. The monthly maximum in OM occurs during May, one month after the peak in nss-SO and two months after that of elemental carbon (EC). Winter (DJF), spring (MAM), summer and fall (SON) values of OM/nss-SO are 26 %, 28 %, 107 % and 39 %, respectively, and overall about 40 % of the weekly variability in the OM is associated with nss-SO. Respective study-averaged concentrations of alkane, alcohol, acid, amine and carbonyl groups are 57 ng m, 24 ng m, 23 ng m, 16 ng m and 11 ng m, representing 42 %, 22 %, 18 %, 14 % and 5 % of the OM, respectively. Carbonyl groups, detected mostly during spring, may have a connection with snow chemistry. The seasonally highest O/C occurs during winter (0.85) and the lowest O/C is during spring (0.51); increases in O/C are largely due to increases in alcohol groups. During winter, more than 50 % of the alcohol groups are associated with primary marine emissions, consistent with Shaw et al. (2010) and Frossard et al. (2011). A secondary marine connection, rather than a primary source, is suggested for the highest and most persistence O/C observed during the coolest and cleanest summer (2013), when alcohol and acid groups made up 63% of the OM. A secondary marine source may be a general feature of the summer OM, but higher contributions from alkane groups to OM during the warmer summers of 2012 (53 %) and 2014 (50 %) were likely due to increased contributions from combustion sources. Evidence for significant contributions from biomass burning (BB) was present in 4 % of the weeks. During the dark months (NDJF), 29 %, 28 % and 14 % of the nss-SO, EC and OM were associated with transport times over the gas flaring region of Northern Russia and other parts of Eurasia. During spring, those percentages drop to 11 % and 8 % for nss-SO and EC, respectively, and there is no association of OM. Large percentages of the Arctic Haze characterized at Alert likely have origins farther than 10 days transport time and may be from outside of the Eurasian region. Possible sources of unusually high nss-SO and OM during September–October, 2014 are volcanic emissions or the ’ area of the Northwest Territories, Canada.