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@ARTICLE{Hottmann:890288,
author = {Hottmann, Bettina and Hafermann, Sascha and Tomsche, Laura
and Marno, Daniel and Martinez, Monica and Harder, Hartwig
and Pozzer, Andrea and Neumaier, Marco and Zahn, Andreas and
Bohn, Birger and Stratmann, Greta and Ziereis, Helmut and
Lelieveld, Jos and Fischer, Horst},
title = {{I}mpact of the {S}outh {A}sian monsoon outflow on
atmospheric hydroperoxides in the upper troposphere},
journal = {Atmospheric chemistry and physics},
volume = {20},
number = {21},
issn = {1680-7324},
address = {Katlenburg-Lindau},
publisher = {EGU},
reportid = {FZJ-2021-00869},
pages = {12655 - 12673},
year = {2020},
abstract = {During the OMO (Oxidation Mechanism Observation) mission,
trace gas measurements were performed on board the HALO
(High Altitude Long Range) research aircraft in summer 2015
in order to investigate the outflow of the South Asian
summer monsoon and its influence on the composition of the
Asian monsoon anticyclone (AMA) in the upper troposphere
over the eastern Mediterranean and the Arabian Peninsula.
This study focuses on in situ observations of hydrogen
peroxide (H2O2obs) and organic hydroperoxides (ROOHobs) as
well as their precursors and loss processes. Observations
are compared to photostationary-state (PSS) calculations of
H2O2PSS and extended by a separation of ROOHobs into methyl
hydroperoxide (MHPPSS) and inferred unidentified
hydroperoxide (UHPPSS) mixing ratios using PSS calculations.
Measurements are also contrasted to simulations with the
general circulation ECHAM–MESSy for Atmospheric Chemistry
(EMAC) model. We observed enhanced mixing ratios of H2O2obs
$(45 \%),$ MHPPSS $(9 \%),$ and UHPPSS $(136 \%)$ in
the AMA relative to the northern hemispheric background.
Highest concentrations for H2O2obs and MHPPSS of 211 and
152 ppbv, respectively, were found in the tropics outside
the AMA, while for UHPPSS, with 208 pptv, highest
concentrations were found within the AMA. In general, the
observed concentrations are higher than steady-state
calculations and EMAC simulations by a factor of 3 and 2,
respectively. Especially in the AMA, EMAC underestimates the
H2O2EMAC (medians: 71 pptv vs. 164 pptv) and ROOHEMAC
(medians: 25 pptv vs. 278 pptv) mixing ratios.
Longitudinal gradients indicate a pool of hydroperoxides
towards the center of the AMA, most likely associated with
upwind convection over India. This indicates main
contributions of atmospheric transport to the local budgets
of hydroperoxides along the flight track, explaining strong
deviations from steady-state calculations which only account
for local photochemistry. Underestimation of H2O2EMAC by
approximately a factor of 2 in the Northern Hemisphere (NH)
and the AMA and overestimation in the Southern Hemisphere
(SH; factor 1.3) are most likely due to uncertainties in the
scavenging efficiencies for individual hydroperoxides in
deep convective transport to the upper troposphere,
corroborated by a sensitivity study. It seems that the
observed excess UHPPSS is excess MHP transported to the west
from an upper tropospheric source related to convection in
the summer monsoon over Southeast Asia.},
cin = {IEK-8},
ddc = {550},
cid = {I:(DE-Juel1)IEK-8-20101013},
pnm = {243 - Tropospheric trace substances and their
transformation processes (POF3-243)},
pid = {G:(DE-HGF)POF3-243},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000584387800003},
doi = {10.5194/acp-20-12655-2020},
url = {https://juser.fz-juelich.de/record/890288},
}