Microlayer source of oxygenated volatile organic compounds in the summertime marine Arctic boundary layer

Mungall, Emma L.; Abbatt, Jonathan P. D.; Wentzell, Jeremy J. B.; Lee, Alex K. Y.; Thomas, Jennie L.; Blais, Marjolaine; Gosselin, Michel; Miller, Lisa A.; Papakyriakou, Tim; Willis, Megan D.; Liggio, John

doi:10.1073/pnas.1620571114

Cited by 121 publications

(157 citation statements)

References 69 publications

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“…For the summer of 2013, the association of alcohol groups with lower concentrations of ss-Na + and higher concentrations of MSA suggests a stronger connection with secondary marine sources. That result may be consistent with Mungall et al (2017) who found evidence for summertime secondary marine precursors in the form of oxygenated VOCs possibly due to photochemical reactions at the surface of waters in the NARES Strait that divides Ellesmere Island and Greenland.…”

Section: Chemical Component Correlationssupporting

confidence: 92%

“…Their organic functional group (OFG) analyses showed the winterspring OM consisted primarily of alkane and carboxylic acid groups from combustion sources and carbohydrate-like substances hypothesized to be from sea spray in spring and frost flower formation associated with new sea ice formation in winter (Shaw et al, 2010;Russell et al, 2010). Marine sources further contribute to OM in spring and summer through emissions of biogenic volatile organic compounds (BVOCs; e.g., isoprene and terpenes) that are oxidized in the atmosphere (Fu et al, 2009a), oxygenated VOCs (OVOCs; Mungall et al, 2017) and trimethylamines (Köllner et al, 2017) as well as from direct emissions of sea spray Frossard et al, 2011Frossard et al, , 2014. During winter and early spring, much of the OM may come from Eurasian fossil fuel sources (e.g., Behrenfeldt et al, 2008;Nguyen et al, 2013;Barrett et al, 2015), and it is mixed with sulfates and nitrates (Weinbruch et al, 2012).…”

Section: Introductionmentioning

confidence: 99%

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Organic functional groups in the submicron aerosol at 82.5° N, 62.5° W from 2012 to 2014

et al. 2018

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Abstract. 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 (OM) concentrations but higher ratios of OM to non-sea-salt sulfate mass concentrations (nss-SO = 4 ) accompany smaller particles during the summer (JJA). Conversely, higher OM but lower OM / nss-SO = 4 accompany larger particles during winter-spring. OM ranges from 7 to 460 ng m −3 , and the study average is 129 ng m −3 . The monthly maximum in OM occurs during May, 1 month after the peak in nss-SO = 4 and 2 months after that of elemental carbon (EC). Winter (DJF), spring (MAM), summer and fall (SON) values of OM / nss-SO = 4 are 26, 28, 107 and 39 %, respectively, and overall about 40 % of the weekly variability in the OM is associated with nss-SO = 4 . Respective study-averaged concentrations of alkane, alcohol, acid, amine and carbonyl groups are 57, 24, 23, 15 and 11 ng m −3 , 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 persistent 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 = 4 , 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 dropped to 11 % for each of nss-SO = 4 and EC values, respectively, and there is no association of OM.

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Section: Chemical Component Correlationssupporting

confidence: 92%

Section: Introductionmentioning

confidence: 99%

Organic functional groups in the submicron aerosol at 82.5° N, 62.5° W from 2012 to 2014

et al. 2018

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“…The prevalence of the factor in the fall and spring, before polar sunset and after polar sunrise, would support a photochemical source. Furthermore, summertime measurements of Arctic atmospheric samples by Mungall et al (2017) also showed high levels of formic and acetic acid and hypothesized an oceanic microlayer photochemical source. Again, the temporal trend of Factor 4 as well as the Atlantic Ocean source location would support this possibility.…”

Section: Factor 4: Carboxylic Acidsmentioning

confidence: 97%

Temporally delineated sources of major chemical species in high Arctic snow

et al. 2018

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Abstract. Long-range transport of aerosol from lower latitudes to the high Arctic may be a significant contributor to climate forcing in the Arctic. To identify the sources of key contaminants entering the Canadian High Arctic an intensive campaign of snow sampling was completed at Alert, Nunavut, from September 2014 to June 2015. Fresh snow samples collected every few days were analyzed for black carbon, major ions, and metals, and this rich data set provided an opportunity for a temporally refined source apportionment of snow composition via positive matrix factorization (PMF) in conjunction with FLEXPART (FLEXible PARTicle dispersion model) potential emission sensitivity analysis. Seven source factors were identified: sea salt, crustal metals, black carbon, carboxylic acids, nitrate, noncrustal metals, and sulfate. The sea salt and crustal factors showed good agreement with expected composition and primarily northern sources. High loadings of V and Se onto Factor 2, crustal metals, was consistent with expected elemental ratios, implying these metals were not primarily anthropogenic in origin. Factor 3, black carbon, was an acidic factor dominated by black carbon but with some sulfate contribution over the winter-haze season. The lack of K + associated with this factor, a Eurasian source, and limited known forest fire events coincident with this factor's peak suggested a predominantly anthropogenic combustion source. Factor 4, carboxylic acids, was dominated by formate and acetate with a moderate correlation to available sunlight and an oceanic and North American source. A robust identification of this factor was not possible; however, atmospheric photochemical reactions, ocean microlayer reaction, and biomass burning were explored as potential contributors. Factor 5, nitrate, was an acidic factor dominated by NO − 3 , with a likely Eurasian source and mid-winter peak. The isolation of NO − 3 on a separate factor may reflect its complex atmospheric processing, though the associated source region suggests possibly anthropogenic precursors. Factor 6, non-crustal metals, showed heightened loadings of Sb, Pb, and As, and correlation with other metals traditionally associated with industrial activities. Similar to Factor 3 and 5, this factor appeared to be largely Eurasian in origin. Factor 7, sulfate, was dominated by SO 2− 4 and MS with a fall peak and high acidity. Coincident volcanic activity and northern source regions may suggest a processed SO 2 source of this factor.

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“…DOC was determined using a hightemperature combustion Shimadzu TOC-V CPN Total Organic Carbon Analyzer, as described in detail by Mungall et al (2017). Chl a concentrations an index of phytoplankton biomass, was measured using a 10-AU Turner Designs fluorometer following the acidification method of Parsons et al (1984).…”

Section: Oceanic Measurementsmentioning

confidence: 99%

Frequent ultrafine particle formation and growth in Canadian Arctic marine and coastal environments

et al. 2017

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Abstract. The source strength and capability of aerosol particles in the Arctic to act as cloud condensation nuclei have important implications for understanding the indirect aerosolcloud effect within the polar climate system. It has been shown in several Arctic regions that ultrafine particle (UFP) formation and growth is a key contributor to aerosol number concentrations during the summer. This study uses aerosol number size distribution measurements from shipboard expeditions aboard the research icebreaker CCGS Amundsen in the summers of 2014 and 2016 throughout the Canadian Arctic to gain a deeper understanding of the drivers of UFP formation and growth within this marine boundary layer. UFP number concentrations (diameter > 4 nm) in the range of 10 1 -10 4 cm −3 were observed during the two seasons, with concentrations greater than 10 3 cm −3 occurring more frequently in 2016. Higher concentrations in 2016 were associated with UFP formation and growth, with events occurring on 41 % of days, while events were only observed on 6 % of days in 2014. Assessment of relevant parameters for aerosol nucleation showed that the median condensation sink in this region was approximately 1.2 h −1 in 2016 and 2.2 h −1 in 2014, which lie at the lower end of ranges observed at even the most remote stations reported in the literature. Apparent growth rates of all observed events in both expeditions averaged 4.3 ± 4.1 nm h −1 , in general agreement with other recent studies at similar latitudes. Higher solar radiation, lower cloud fractions, and lower sea ice concentrations combined with differences in the developmental stage and activity of marine microbial communities within the Canadian Arctic were documented and help explain differences between the aerosol measurements made during the 2014 and 2016 expeditions. These findings help to motivate further studies of biosphere-atmosphere interactions within the Arctic marine environment to explain the production of UFP and their growth to sizes relevant for cloud droplet activation.

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Microlayer source of oxygenated volatile organic compounds in the summertime marine Arctic boundary layer

Cited by 121 publications

References 69 publications

Organic functional groups in the submicron aerosol at 82.5° N, 62.5° W from 2012 to 2014

Organic functional groups in the submicron aerosol at 82.5° N, 62.5° W from 2012 to 2014

Temporally delineated sources of major chemical species in high Arctic snow

Frequent ultrafine particle formation and growth in Canadian Arctic marine and coastal environments

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Microlayer source of oxygenated volatile organic compounds in the summertime marine Arctic boundary layer

Cited by 121 publications

References 69 publications

Organic functional groups in the submicron aerosol at 82.5° N, 62.5° W from 2012 to 2014

Organic functional groups in the submicron aerosol at 82.5° N, 62.5° W from 2012 to 2014

Temporally delineated sources of major chemical species in high Arctic snow

Frequent ultrafine particle formation and growth in Canadian Arctic marine and coastal environments

Contact Info

Product

Resources

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Organic functional groups in the submicron aerosol at 82.5° N, 62.5° W from 2012 to 2014

Organic functional groups in the submicron aerosol at 82.5° N, 62.5° W from 2012 to 2014