Source and variability of formaldehyde (HCHO) at northern high latitudes: an integrated satellite, aircraft, and model study
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...
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Veröffentlicht in: | Atmospheric chemistry and physics 2022-06, Vol.22 (11), p.7163-7178 |
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Zusammenfassung: | 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. |
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ISSN: | 1680-7324 1680-7316 1680-7324 |
DOI: | 10.5194/acp-22-7163-2022 |