Role of convection in redistributing formaldehyde to the upper troposphere over North America and the North Atlantic during the summer 2004 INTEX campaign

Autor: Xinrong Ren, Gao Chen, Michael Porter, R. Shetter, Antony D. Clarke, Cameron S. McNaughton, J. Snow, James H. Crawford, Stephanie A. Vay, Kenneth E. Pickering, Ronald C. Cohen, Petter Weibring, Glen W. Sachse, Timothy H. Bertram, S. Kim, Dylan B. Millet, Hanwant B. Singh, Donald R. Blake, Nicola J. Blake, Alan Fried, Jennifer R. Olson, Brian G. Heikes, Lee Thornhill, James Walega, William H. Brune, Frank K. Tittel, Haiwei Shen, Glenn S. Diskin, G. Huey, Chad Roller, Jeremy Halland, Dirk Richter, Daniel O'Sullivan, Samuel R. Hall, Melody A. Avery, Bruce E. Anderson, Henry E. Fuelberg, James R. Podolske
Rok vydání: 2008
Předmět:
Zdroj: Journal of Geophysical Research. 113
ISSN: 0148-0227
DOI: 10.1029/2007jd009760
Popis: Measurements of CH2O from a tunable diode laser absorption spectrometer (TDLAS) were acquired onboard the NASA DC-8 during the summer 2004 INTEX-NA (Intercontinental Chemical Transport Experiment - North America) campaign to test our understanding of convection and production mechanisms in the upper troposphere (UT, 6-12-km) over continental North America and the North Atlantic Ocean. Point-by-point comparisons with box model calculations, when MHP (CH3OOH) measurements were available for model constraint, resulted in a median CH2O measurement/model ratio of 0.91 in the UT. Multiple tracers were used to arrive at a set of UT CH2O background and perturbed air mass periods, and 46% of the TDLAS measurements fell within the latter category. At least 66% to 73% of these elevated UT observations were caused by enhanced production from CH2O precursors rather than direct transport of CH2O from the boundary layer. This distinction is important, since the effects from the former can last for over a week or more compared to one day or less in the case of convective transport of CH2O itself. In general, production of CH2O from CH4 was found to be the dominant source term, even in perturbed air masses. This was followed by production from MHP, methanol, PAN type compounds, and ketones, in descending order of their contribution. In the presence of elevated NO from lightning and potentially from the stratosphere, there was a definite trend in the CH2O discrepancy, which for the highest NO mixing ratios produced a median CH2O measurement/model ratio of 3.9 in the 10-12-km range. Discrepancies in CH2O and HO2 in the UT with NO were highly correlated and this provided further information as to the possible mechanism(s) responsible. These discrepancies with NO are consistent with additional production sources of both gases involving CH3O2 + NO reactions, most likely caused by unmeasured hydrocarbons.
Databáze: OpenAIRE
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