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@ARTICLE{Cho:891564,
author = {Cho, Changmin and Hofzumahaus, Andreas and Fuchs, Hendrik
and Dorn, Hans-Peter and Glowania, Marvin and Holland, Frank
and Rohrer, Franz and Vardhan, Vaishali and Kiendler-Scharr,
Astrid and Wahner, Andreas and Novelli, Anna},
title = {{C}haracterization of a chemical modulation reactor ({CMR})
for the measurement of atmospheric concentrations of
hydroxyl radicals with a laser-induced fluorescence
instrument},
journal = {Atmospheric measurement techniques},
volume = {14},
number = {3},
issn = {1867-8548},
address = {Katlenburg-Lindau},
publisher = {Copernicus},
reportid = {FZJ-2021-01589},
pages = {1851 - 1877},
year = {2021},
abstract = {Precise and accurate hydroxyl radical (OH) measurements are
essential to investigate mechanisms for oxidation and
transformation of trace gases and processes leading to the
formation of secondary pollutants like ozone (O3) in the
troposphere. Laser-induced fluorescence (LIF) is a widely
used technique for the measurement of ambient OH radicals
and was used for the majority of field campaigns and chamber
experiments. Recently, most LIF instruments in use for
atmospheric measurements of OH radicals introduced chemical
modulation to separate the ambient OH radical concentration
from possible interferences by chemically removing ambient
OH radicals before they enter the detection cell (Mao et
al., 2012; Novelli et al., 2014a). In this study, we
describe the application and characterization of a chemical
modulation reactor (CMR) applied to the Forschungszentrum
Jülich LIF (FZJ-LIF) instrument in use at the atmospheric
simulation chamber SAPHIR (Simulation of Atmospheric
PHotochemistry In a large Reaction Chamber). Besides
dedicated experiments in synthetic air, the new technique
was extensively tested during the year-round Jülich
Atmospheric Chemistry Project (JULIAC) campaign, in which
ambient air was continuously flowed into the SAPHIR chamber.
It allowed for performing OH measurement comparisons with
differential optical absorption spectroscopy (DOAS) and
investigation of interferences in a large variety of
chemical and meteorological conditions. Good agreement was
obtained in the LIF–DOAS intercomparison within
instrumental accuracies $(18 \%$ for LIF and $6.5 \%$
for DOAS) which confirms that the new chemical modulation
system of the FZJ-LIF instrument is suitable for measurement
of interference-free OH concentrations under the conditions
of the JULIAC campaign (rural environment). Known
interferences from O3+H2O and the nitrate radical (NO3) were
quantified with the CMR in synthetic air in the chamber and
found to be 3.0×105 and 0.6×105 cm−3, respectively,
for typical ambient-air conditions (O3=50 ppbv, H2O =
$1 \%$ and NO3=10 pptv). The interferences measured in
ambient air during the JULIAC campaign in the summer season
showed a median diurnal variation with a median maximum
value of 0.9×106 cm−3 during daytime and a median
minimum value of 0.4×106 cm−3 at night. The highest
interference of 2×106 cm−3 occurred in a heat wave from
22 to 29 August, when the air temperature and ozone
increased to 40 ∘C and 100 ppbv, respectively. All
observed interferences could be fully explained by the known
O3+H2O interference, which is routinely corrected in FZJ-LIF
measurements when no chemical modulation is applied. No
evidence for an unexplained interference was found during
the JULIAC campaign.A chemical model of the CMR was
developed and applied to estimate the possible perturbation
of the OH transmission and scavenging efficiency by reactive
atmospheric trace gases. These can remove OH by gas phase
reactions in the CMR or produce OH by non-photolytic
reactions, most importantly by the reaction of ambient HO2
with NO. The interfering processes become relevant at high
atmospheric OH reactivities. For the conditions of the
JULIAC campaign with OH reactivities below 20 s−1, the
influence on the determination of ambient OH concentrations
was small (on average: $2 \%).$ However, in environments
with high OH reactivities, such as in a rain forest or
megacity, the expected perturbation in the currently used
chemical modulation reactor could be large (more than a
factor of 2). Such perturbations need to be carefully
investigated and corrected for the proper evaluation of OH
concentrations when applying chemical scavenging. This
implies that chemical modulation, which was developed to
eliminate interferences in ambient OH measurements, itself
can be subject to interferences that depend on ambient
atmospheric conditions.},
cin = {IEK-8},
ddc = {550},
cid = {I:(DE-Juel1)IEK-8-20101013},
pnm = {211 - Die Atmosphäre im globalen Wandel (POF4-211)},
pid = {G:(DE-HGF)POF4-211},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000626739200002},
doi = {10.5194/amt-14-1851-2021},
url = {https://juser.fz-juelich.de/record/891564},
}