Composition, concentration, and oxidant reactivity of sesquiterpenes in the southeastern US

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dc.contributor.authorFrazier, Grahamen
dc.contributor.authorMcGlynn, Deborah F.en
dc.contributor.authorBarry, Laura E.en
dc.contributor.authorLerdau, Manuelen
dc.contributor.authorPusede, Sally E.en
dc.contributor.authorIsaacman-VanWertz, Gabrielen
dc.coverage.countryUnited Statesen
dc.date.accessioned2022-10-18T13:13:12Zen
dc.date.available2022-10-18T13:13:12Zen
dc.date.issued2022-09-15en
dc.description.abstractBiogenic volatile organic compounds (BVOCs) contribute the majority of reactive organic carbon to the atmosphere and lead to aerosol formation through reaction with atmospheric oxidants including ozone and hydroxyl radicals. One class of BVOCs, sesquiterpenes, have a high reactivity with ozone but exist at lower concentrations compared to other BVOCs, and there are relatively few measurements of their concentrations in different environments or their importance in the atmospheric oxidant budget. To help close this knowledge gap, we examine concentrations of isomer-resolved sesquiterpene concentrations collected hourly at two sites in Virginia that are representative of different ecosystems in the southeastern US. Sesquiterpene concentrations are presented and discussed in relation to their diurnal patterns and used to estimate their contribution to reactivity with common gas-phase oxidants. Twenty-four sesquiterpenes were identified at the sites, eleven of which were observed at both sites. Total sesquiterpene concentrations were found to range between 0.8 and 2 ppt with no single isomer dominating throughout. Hydroxyl activity is similarly diverse, with no particular isomer dominating activity at either site. Ozone reactivity, however, was found to be dominated (similar to 3/4 total reactivity) by beta-caryophyllene and humulene despite these compounds representing roughly only 10% of total sesquiterpene mass, highlighting their importance as the major driver of sesquiterpene-ozone reactivity. Average reaction rate constants for sesquiterpenes with ozone and hydroxyl radicals were calculated for both sites as a method to simplify future atmospheric modelling concerning sesquiterpenes. This work provides broad insight into the composition and impacts of sesquiterpenes, suggesting that sesquiterpene composition is relatively similar between sites. Furthermore, while the calculated average sesquiterpene-ozone reaction rate constants are at least an order of magnitude higher than that of more prevalent BVOC classes (isoprene and monoterpenes), their low concentrations suggest their impacts on atmospheric reactivity are expected to be limited to periods of high emissions.en
dc.description.notesThis research was funded by the National Science Foundation (AGS 1837882 and AGS 1837891). Tower maintenance and operation were supported in part by the Pace Endowment. Deborah F. McGlynn and Laura E. R. Barry were supported in part by Virginia Space Grant Consortium Graduate Research Fellowships. Graham Frazier was supported in part by the Edna Bailey Sussman Foundation Internship. We would like to thank the reviewers for help in strengthening the presentation of this paper. In particular, we would like to thank reviewer 3 for their advice on formatting of Fig. 2 to better display the data.en
dc.description.sponsorshipNational Science Foundation [AGS 1837882, AGS 1837891]; Pace Endowment; Virginia Space Grant Consortium Graduate Research Fellowships; Edna Bailey Sussman Foundation Internshipen
dc.description.versionPublished versionen
dc.format.mimetypeapplication/pdfen
dc.identifier.doihttps://doi.org/10.1039/d2ea00059hen
dc.identifier.eissn2634-3606en
dc.identifier.issue5en
dc.identifier.urihttp://hdl.handle.net/10919/112186en
dc.identifier.volume2en
dc.language.isoenen
dc.publisherRoyal Society of Chemistryen
dc.rightsCreative Commons Attribution-NonCommercial 4.0 Internationalen
dc.rights.urihttp://creativecommons.org/licenses/by-nc/4.0/en
dc.subjectvolatile organic-compoundsen
dc.subjectphase tropospheric chemistryen
dc.subjectaerosol formationen
dc.subjectatmospheric sesquiterpenesen
dc.subjectemission ratesen
dc.subjectrate constantsen
dc.subjectgasen
dc.subjectforesten
dc.subjectozoneen
dc.subjectvegetationen
dc.titleComposition, concentration, and oxidant reactivity of sesquiterpenes in the southeastern USen
dc.title.serialEnvironmental Science-Atmospheresen
dc.typeArticle - Refereeden
dc.type.dcmitypeTexten

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