Mapping hydroxyl variability throughout the global remote troposphere via synthesis of airborne and satellite formaldehyde observations.

作者: Glenn M. Wolfe , Julie M. Nicely , Jason M. St. Clair , Thomas F. Hanisco , Jin Liao

DOI: 10.1073/PNAS.1821661116

关键词:

摘要: The hydroxyl radical (OH) fuels tropospheric ozone production and governs the lifetime of methane many other gases. Existing methods to quantify global OH are limited annual global-to-hemispheric averages. Finer resolution is essential for isolating model deficiencies building process-level understanding. In situ observations from Atmospheric Tomography (ATom) mission demonstrate that remote tightly coupled loss formaldehyde (HCHO), a major hydrocarbon oxidation product. Synthesis this relationship with satellite-based HCHO retrievals model-derived frequencies yields map total-column abundance throughout troposphere (up 70% mass) over first two ATom missions (August 2016 February 2017). This dataset offers unique insights on near-global oxidizing capacity. exhibits significant seasonality within individual hemispheres, but domain mean concentration nearly identical both seasons (1.03 ± 0.25 × 106 cm−3), biseasonal average North/South Hemisphere ratio 0.89 0.06, consistent balance sources sinks across troposphere. Regional phenomena also highlighted, such as 10-fold depression in Tropical West Pacific enhancements East South Atlantic. method complementary budget-based constraints can help elucidate spatial temporal variability loss.

参考文章(53)
R. E. Huie, V. L. Orkin, M. J. Kurylo, D. M. Wilmouth, J. R. Barker, C. E. Kolb, J. P. D. Abbatt, S. P. Sander, J. B. Burkholder, P. H. Wine, Chemical Kinetics and Photochemical Data for Use in Atmospheric Studies: Evaluation Number 18 Jet Propulsion Laboratory. ,(2015)
Paul O Wennberg, Synte Peacock, James T Randerson, Rainer Bleck, Recent changes in the air‐sea gas exchange of methyl chloroform Geophysical Research Letters. ,vol. 31, ,(2004) , 10.1029/2004GL020476
SA Montzka, CM Spivakovsky, JH Butler, JW Elkins, LT Lock, DJ Mondeel, New observational constraints for atmospheric hydroxyl on global and hemispheric scales Science. ,vol. 288, pp. 500- 503 ,(2000) , 10.1126/SCIENCE.288.5465.500
Derek York, LEAST-SQUARES FITTING OF A STRAIGHT LINE Canadian Journal of Physics. ,vol. 44, pp. 1079- 1086 ,(1966) , 10.1139/P66-090
Daniel Stone, Lisa K. Whalley, Dwayne E. Heard, Tropospheric OH and HO2 radicals: field measurements and model comparisons. Chemical Society Reviews. ,vol. 41, pp. 6348- 6404 ,(2012) , 10.1039/C2CS35140D
R. S. Gao, K. H. Rosenlof, D. W. Fahey, P. O. Wennberg, E. J. Hintsa, T. F. Hanisco, OH in the tropical upper troposphere and its relationships to solar radiation and reactive nitrogen Journal of Atmospheric Chemistry. ,vol. 71, pp. 55- 64 ,(2014) , 10.1007/S10874-014-9280-2
R. PRINN, D. CUNNOLD, R. RASMUSSEN, P. SIMMONDS, F. ALYEA, A. CRAWFORD, P. FRASER, R. ROSEN, Atmospheric Trends in Methylchloroform and the Global Average for the Hydroxyl Radical Science. ,vol. 238, pp. 945- 950 ,(1987) , 10.1126/SCIENCE.238.4829.945
M. Rex, I. Wohltmann, T. Ridder, R. Lehmann, K. Rosenlof, P. Wennberg, D. Weisenstein, J. Notholt, K. Krüger, V. Mohr, S. Tegtmeier, A tropical West Pacific OH minimum and implications for stratospheric composition Atmospheric Chemistry and Physics. ,vol. 14, pp. 4827- 4841 ,(2014) , 10.5194/ACP-14-4827-2014
Maarten Krol, Jos Lelieveld, Can the variability in tropospheric OH be deduced from measurements of 1,1,1‐trichloroethane (methyl chloroform)? Journal of Geophysical Research. ,vol. 108, pp. 4125- ,(2003) , 10.1029/2002JD002423