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@ARTICLE{Jin:1017878,
author = {Jin, Lixu and Permar, Wade and Selimovic, Vanessa and
Ketcherside, Damien and Yokelson, Robert J. and Hornbrook,
Rebecca S. and Apel, Eric C. and Ku, I-Ting and Collett Jr.,
Jeffrey L. and Sullivan, Amy P. and Jaffe, Daniel A. and
Pierce, Jeffrey R. and Fried, Alan and Coggon, Matthew M.
and Gkatzelis, Georgios and Warneke, Carsten and Fischer,
Emily V. and Hu, Lu},
title = {{C}onstraining emissions of volatile organic compounds from
western {US} wildfires with {WE}-{CAN} and {FIREX}-{AQ}
airborne observations},
journal = {Atmospheric chemistry and physics},
volume = {23},
number = {10},
issn = {1680-7316},
address = {Katlenburg-Lindau},
publisher = {EGU},
reportid = {FZJ-2023-04390},
pages = {5969 - 5991},
year = {2023},
abstract = {The impact of biomass burning (BB) on the atmospheric
burden of volatile organic compounds (VOCs) is highly
uncertain. Here we apply the GEOS-Chem chemical transport
model (CTM) to constrain BB emissions in the western USA at
∼ 25 km resolution. Across three BB emission
inventories widely used in CTMs, the inventory–inventory
comparison suggests that the totals of 14 modeled BB VOC
emissions in the western USA agree with each other within
$30 \%–40 \%.$ However, emissions for individual VOCs
can differ by a factor of 1–5, driven by the regionally
averaged emission ratios (ERs, reflecting both assigned ERs
for specific biome and vegetation classifications) across
the three inventories. We further evaluate GEOS-Chem
simulations with aircraft observations made during WE-CAN
(Western Wildfire Experiment for Cloud Chemistry, Aerosol
Absorption and Nitrogen) and FIREX-AQ (Fire Influence on
Regional to Global Environments and Air Quality) field
campaigns. Despite being driven by different global BB
inventories or applying various injection height
assumptions, the model–observation comparison suggests
that GEOS-Chem simulations underpredict observed vertical
profiles by a factor of 3–7. The model shows small to no
bias for most species in low-/no-smoke conditions. We thus
attribute the negative model biases mostly to underestimated
BB emissions in these inventories. Tripling BB emissions in
the model reproduces observed vertical profiles for primary
compounds, i.e., CO, propane, benzene, and toluene. However,
it shows no to less significant improvements for oxygenated
VOCs, particularly for formaldehyde, formic acid, acetic
acid, and lumped ≥ C3 aldehydes, suggesting the model is
missing secondary sources of these compounds in BB-impacted
environments. The underestimation of primary BB emissions in
inventories is likely attributable to underpredicted amounts
of effective dry matter burned, rather than errors in fire
detection, injection height, or ERs, as constrained by
aircraft and ground measurements. We cannot rule out
potential sub-grid uncertainties (i.e., not being able to
fully resolve fire plumes) in the nested GEOS-Chem which
could explain the negative model bias partially, though
back-of-the-envelope calculation and evaluation using
longer-term ground measurements help support the argument of
the dry matter burned underestimation. The total ERs of the
14 BB VOCs implemented in GEOS-Chem only account for half of
the total 161 measured VOCs (∼ 75 versus
150 ppb ppm−1). This reveals a significant amount of
missing reactive organic carbon in widely used BB emission
inventories. Considering both uncertainties in effective dry
matter burned (× 3) and unmodeled VOCs (× 2), we infer
that BB contributed to $10 \%$ in 2019 and $45 \%$ in
2018 (240 and 2040 Gg C) of the total VOC primary
emission flux in the western USA during these two fire
seasons, compared to only $1 \%–10 \%$ in the standard
GEOS-Chem.},
cin = {IEK-8},
ddc = {550},
cid = {I:(DE-Juel1)IEK-8-20101013},
pnm = {2111 - Air Quality (POF4-211)},
pid = {G:(DE-HGF)POF4-2111},
typ = {PUB:(DE-HGF)16},
UT = {WOS:001000070100001},
doi = {10.5194/acp-23-5969-2023},
url = {https://juser.fz-juelich.de/record/1017878},
}