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DOI10.5194/acp-19-349-2019
ROOOH: A missing piece of the puzzle for OH measurements in low-NO environments?
Fittschen C.; Al Ajami M.; Batut S.; Ferracci V.; Archer-Nicholls S.; Archibald T.A.; Schoemaecker C.
发表日期2019
ISSN16807316
起始页码349
结束页码362
卷号19期号:1
英文摘要Field campaigns have been carried out with the FAGE (fluorescence assay by gas expansion) technique in remote biogenic environments in the last decade to quantify the in situ concentrations of OH, the main oxidant in the atmosphere. These data have revealed concentrations of OH radicals up to a factor of 10 higher than predicted by models, whereby the disagreement increases with decreasing NO concentration. This was interpreted as a major lack in our understanding of the chemistry of biogenic VOCs (volatile organic compounds), particularly isoprene, which are dominant in remote pristine conditions. But interferences in these measurements of unknown origin have also been discovered for some FAGE instruments: using a pre-injector, all ambient OH is removed by fast reaction before entering the FAGE cell, and any remaining OH signal can be attributed to an interference. This technique is now systematically used for FAGE measurements, allowing the reliable quantification of ambient OH concentrations along with the signal due to interference OH. However, the disagreement between modelled and measured high OH concentrations of earlier field campaigns as well as the origin of the now-quantifiable background OH is still not understood. We present in this paper the compelling idea that this interference, and thus the disagreement between model and measurement in earlier field campaigns, might be at least partially due to the unexpected decomposition of a new class of molecule, ROOOH, within the FAGE instruments. This idea is based on experiments, obtained with the FAGE set-up of the University of Lille, and supported by a modelling study. Even though the occurrence of this interference will be highly dependent on the design and measurement conditions of different FAGE instruments, including ROOOH in atmospheric chemistry models might reflect a missing piece of the puzzle in our understanding of OH in clean atmospheres. © Author(s) 2019. This work is distributed under the Creative Commons Attribution 4.0 License.
语种英语
scopus关键词assay; atmospheric chemistry; concentration (composition); fluorescence; hydroxyl radical; measurement method; nitrogen oxides; volatile organic compound
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/144731
作者单位PhysicoChimie des Processus de Combustion et de l'Atmosphère - PC2A, Université Lille, CNRS, UMR 8522, Lille, 59000, France; Department of Chemistry, University of Cambridge, Centre for Atmospheric Science, Lensfield Road, Cambridge, CB2g1EW, United Kingdom; Centre for Environmental and Agricultural Informatics, Cranfield University, College Road, Cranfield, MK43g0AL, United Kingdom; National Centre for Atmospheric Science, Cambridge, CB2g1EW, United Kingdom
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Fittschen C.,Al Ajami M.,Batut S.,et al. ROOOH: A missing piece of the puzzle for OH measurements in low-NO environments?[J],2019,19(1).
APA Fittschen C..,Al Ajami M..,Batut S..,Ferracci V..,Archer-Nicholls S..,...&Schoemaecker C..(2019).ROOOH: A missing piece of the puzzle for OH measurements in low-NO environments?.Atmospheric Chemistry and Physics,19(1).
MLA Fittschen C.,et al."ROOOH: A missing piece of the puzzle for OH measurements in low-NO environments?".Atmospheric Chemistry and Physics 19.1(2019).
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