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@PHDTHESIS{Lohse:256276,
author = {Lohse, Insa Mareike},
title = {{S}pektrale aktinische {F}lussdichten und
{P}hotolysefrequenzen – {U}ntersuchungen in der
atmosphärischen {G}renzschicht und der freien
{T}roposphäre},
volume = {285},
school = {Universität Köln},
type = {Dr.},
address = {Jülich},
publisher = {Forschungszentrum Jülich GmbH Zentralbibliothek, Verlag},
reportid = {FZJ-2015-06240},
isbn = {978-3-95806-086-9},
series = {Schriften des Forschungszentrums Jülich Reihe Energie $\&$
Umwelt / Energy $\&$ Environment},
pages = {VI, 111, VII-XXIII S.},
year = {2015},
note = {Universität Köln, Diss., 2015},
abstract = {Solar UV radiation is driving atmospheric photochemistry
because the photolysis of atmospheric trace gases yields
highly reactive atoms or radicals. Thus, trace gas
concentrations as well as accurate photolysis frequencies
are needed to understand atmospheric photochemical
processes. Especially under varying cloud conditions,
measurements can often not be replaced by radiative transfer
calculations with sufficient accuracy. In this work,
airborne measurements of the separate upwelling and
downwelling components of the actinic flux densities
(280–650 nm) were performed with CCD-spectroradiometers.
For accurate UV measurements a thorough treatment of stray
light was applied for the single monochromator based array
spectrometers. Moreover, the angular sensitivities of the
optical receivers were determined to analyze their influence
under various atmospheric conditions using radiative
transfer calculations of realistic atmospheric radiance
distributions. Corresponding correction factors in the range
of $5\%$ were derived. The overall performance was tested on
the ground by in-field comparisons with a
doublemonochromator reference system and found to have
maximum deviations of $7\%.$ Measurements of the spectral
actinic flux density were performed aboard Zeppelin NT in
the atmospheric boundary layer during the PEGASOS campaign
2012/13 over different parts of Europe. Moreover the
research aircraft HALO was used during the NARVAL campaign
2013/14 for measurements in the upper troposphere and the
lower stratosphere over the Atlantic Ocean. Typical Zeppelin
flight heights ranged from 100m to 900m and flights were
therefore always performed below possible cloud layers. Thus
the measurements were influenced by potentially overlaying
clouds and a small upwelling part of radiation. Radiative
transfer calculations of the downwelling component under the
assumption of clearsky conditions showed good agreement with
the maximum values of the measurements. The upwelling
component of the spectral actinic flux density was
unexpectedly greater than the model results. The reason for
this is unknown and requires further reasearch. Owing to the
typical flight heights of HALO in the range 8–14 km, the
measurements were affected by a high upwelling part of
radiation, especially when flying over clouds. The measured
downwelling components of j(O$^{1}$D) and j(NO$_{2}$) for
all flights and various cloud conditions showed only small
deviations of 4–5\% compared to clearsky model
calculations. Cloud-microphysical properties of underlying
clouds were retrieved for a certain time period of a
HALO-flight using spectral radiance measurements performed
by the Leipzig Institute for Meteorology and were used as
additional input parameters for radiative transfer
calculations of spectral actinic flux densities. The
deviations between model and measurements of up to 40\% for
the upwelling component can partly be attributed to the
geometrical receiving characteristics of the radiance optic.
Comparisons of measured photolysis frequencies and model
values of regional and global chemistry transport models
showed good agreements with small underestimations of
j(NO$_{2}$) by the models in the range of 20\%. For the
PEGASOS campaign the regional EURAD-IM model was found to
overestimate j(O$^{1}$D) significantly due to a low and
constant ozone column in the model. For the NARVAL campaign
good agreement for j(O$^{1}$D) with the global MOZART model,
that uses variable, modelled ozone columns, was obtained.},
cin = {IEK-8},
cid = {I:(DE-Juel1)IEK-8-20101013},
pnm = {243 - Tropospheric trace substances and their
transformation processes (POF3-243) / HITEC - Helmholtz
Interdisciplinary Doctoral Training in Energy and Climate
Research (HITEC) (HITEC-20170406)},
pid = {G:(DE-HGF)POF3-243 / G:(DE-Juel1)HITEC-20170406},
typ = {PUB:(DE-HGF)11 / PUB:(DE-HGF)3},
url = {https://juser.fz-juelich.de/record/256276},
}