Tunable diode laser measurements of formaldehyde during the TOPSE 2000 study: Distributions, trends, and model comparisons

Authors

Alan Fried
Yuhang Wang
Chris Cantrell
Bryan Wert
James Walega
Brian Ridley
Elliot Atlas
Rick Shetter
Barry Lefer
M. T. Coffey
Jim Hannigan
Donald Blake
Nicola Blake
Simone Meinardi
bob Talbot
Jack Dibb
Eric Scheuer
Oliver Wingenter
Julie Snow, University of Rhode Island
Brian G. Heikes, University of Rhode IslandFollow
Dieter Ehhalt

Document Type

Article

Date of Original Version

2003

Department

Oceanography

Abstract

Airborne measurements of formaldehyde (CH₂O) were acquired employing tunable diode laser absorption spectroscopy (TDLAS) during the 2000 Tropospheric Ozone Production About the Spring Equinox (TOPSE) study. This study consisted of seven deployments spanning the time period from 4 February to 23 May 2000 and covered a wide latitudinal band from 40°N to 85°N. The median measured CH₂O concentrations, with a few exceptions, did not show any clear temporal trends from February to May in each of five altitude and three latitude bins examined. Detailed measurement–model comparisons were carried out using a variety of approaches employing two different steady state models. Because recent emissions of CH₂O and/or its precursors often result in model underpredictions, background conditions were identified using a number of chemical tracers. For background conditions at temperatures warmer than −45°C, the measurement–model agreement on average ranged between −13% and +5% (measurement–model/measurement), which corresponded to mean and median (measurement–model) differences of 3 ± 69 and −6 parts per trillion by volume (pptv), respectively. At very low temperatures starting at around −45°C, significant and persistent (measurement–model) differences were observed from February to early April from southern Canada to the Arctic Ocean in the 6–8 km altitude range. In such cases, measured CH₂O was as much as 392 pptv higher than modeled, and the median difference was 132 pptv (83%). Low light conditions as well as cold temperatures may be important in this effect. A number of possible mechanisms involving the reaction of CH₃O₂ with HO₂ to produce CH₂O directly were investigated, but in each case the discrepancy was only minimally reduced. Other possibilities were also considered but in each case there was no compelling evidence to support any of the hypotheses. Whatever the cause, the elevated CH₂O concentrations significantly impact upper tropospheric HO_x levels at high latitudes (>57°N) in the February–April time frame.

Citation/Publisher Attribution

Fried, A., et al. (2003), Tunable diode laser measurements of formaldehyde during the TOPSE 2000 study: Distributions, trends, and model comparisons, J. Geophys. Res., 108, 8365, doi: 10.1029/2002JD002208, D4.

Available at: https://doi.org/10.1029/2002JD002208