TY - JOUR
T1 - Source and variability of formaldehyde (HCHO) at northern high latitudes
T2 - An integrated satellite, aircraft, and model study
AU - Zhao, Tianlang
AU - Mao, Jingqiu
AU - Simpson, William R.
AU - De Smedt, Isabelle
AU - Zhu, Lei
AU - Hanisco, Thomas F.
AU - Wolfe, Glenn M.
AU - St. Clair, Jason M.
AU - González Abad, Gonzalo
AU - Nowlan, Caroline R.
AU - Barletta, Barbara
AU - Meinardi, Simone
AU - Blake, Donald R.
AU - Apel, Eric C.
AU - Hornbrook, Rebecca S.
N1 - Publisher Copyright:
© 2022 Tianlang Zhao et al.
PY - 2022/6/3
Y1 - 2022/6/3
N2 - Here we use satellite observations of formaldehyde (HCHO) vertical column densities (VCD) from the TROPOspheric Monitoring Instrument (TROPOMI), aircraft measurements, combined with a nested regional chemical transport model (GEOS-Chem at 0.5×0.625 resolution), to better understand the variability and sources of summertime HCHO in Alaska. We first evaluate GEOS-Chem with in-situ airborne measurements during the Atmospheric Tomography Mission 1 (ATom-1) aircraft campaign. We show reasonable agreement between observed and modeled HCHO, isoprene, monoterpenes and the sum of methyl vinyl ketone and methacrolein (MVK+MACR) in the continental boundary layer. In particular, HCHO profiles show spatial homogeneity in Alaska, suggesting a minor contribution of biogenic emissions to HCHO VCD. We further examine the TROPOMI HCHO product in Alaska in summer, reprocessed by GEOS-Chem model output for a priori profiles and shape factors. For years with low wildfire activity (e.g., 2018), we find that HCHO VCDs are largely dominated by background HCHO (58%-71%), with minor contributions from wildfires (20%-32%) and biogenic VOC emissions (8%-10%). For years with intense wildfires (e.g., 2019), summertime HCHO VCD is dominated by wildfire emissions (50%-72%), with minor contributions from background (22%-41%) and biogenic VOCs (6%-10%). In particular, the model indicates a major contribution of wildfires from direct emissions of HCHO, instead of secondary production of HCHO from oxidation of larger VOCs. We find that the column contributed by biogenic VOC is often small and below the TROPOMI detection limit, in part due to the slow HCHO production from isoprene oxidation under low NOx conditions. This work highlights challenges for quantifying HCHO and its precursors in remote pristine regions.
AB - Here we use satellite observations of formaldehyde (HCHO) vertical column densities (VCD) from the TROPOspheric Monitoring Instrument (TROPOMI), aircraft measurements, combined with a nested regional chemical transport model (GEOS-Chem at 0.5×0.625 resolution), to better understand the variability and sources of summertime HCHO in Alaska. We first evaluate GEOS-Chem with in-situ airborne measurements during the Atmospheric Tomography Mission 1 (ATom-1) aircraft campaign. We show reasonable agreement between observed and modeled HCHO, isoprene, monoterpenes and the sum of methyl vinyl ketone and methacrolein (MVK+MACR) in the continental boundary layer. In particular, HCHO profiles show spatial homogeneity in Alaska, suggesting a minor contribution of biogenic emissions to HCHO VCD. We further examine the TROPOMI HCHO product in Alaska in summer, reprocessed by GEOS-Chem model output for a priori profiles and shape factors. For years with low wildfire activity (e.g., 2018), we find that HCHO VCDs are largely dominated by background HCHO (58%-71%), with minor contributions from wildfires (20%-32%) and biogenic VOC emissions (8%-10%). For years with intense wildfires (e.g., 2019), summertime HCHO VCD is dominated by wildfire emissions (50%-72%), with minor contributions from background (22%-41%) and biogenic VOCs (6%-10%). In particular, the model indicates a major contribution of wildfires from direct emissions of HCHO, instead of secondary production of HCHO from oxidation of larger VOCs. We find that the column contributed by biogenic VOC is often small and below the TROPOMI detection limit, in part due to the slow HCHO production from isoprene oxidation under low NOx conditions. This work highlights challenges for quantifying HCHO and its precursors in remote pristine regions.
UR - https://www.scopus.com/pages/publications/85131820511
U2 - 10.5194/acp-22-7163-2022
DO - 10.5194/acp-22-7163-2022
M3 - Article
AN - SCOPUS:85131820511
SN - 1680-7316
VL - 22
SP - 7163
EP - 7178
JO - Atmospheric Chemistry and Physics
JF - Atmospheric Chemistry and Physics
IS - 11
ER -