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@PHDTHESIS{Fuchs:55628,
author = {Fuchs, Hendrik},
title = {{M}easurement of {P}eroxy {R}adicals using
{L}aser-{I}nduced {F}luorescence {T}echnique},
volume = {72},
issn = {1433-5530},
school = {Humboldt-Universität Berlin},
type = {Dr. (Univ.)},
address = {Jülich},
publisher = {Forschungszentrum Jülich GmbH Zentralbibliothek, Verlag},
reportid = {PreJuSER-55628},
isbn = {3-89336-467-6},
series = {Schriften des Forschungszentrums Jülich. Reihe Umwelt /
Environment},
pages = {VI, 141 S.},
year = {2006},
note = {Record converted from VDB: 12.11.2012;
Humboldt-Universität Berlin, Diss., 2006},
abstract = {Peroxy radicals are produced during the photochemical
degradation of volatile organic compounds (VOCs) in the
atmosphere. They are part of the catalytic radical cycle
initiated by hydroxyl radicals (OH) in which hydrocarbons
are oxidized leading to the removal of pollutants. The
reaction of peroxy radicals with nitrogen monoxide (NO) in
conjunction with the photochemical cycling of nitrogen
dioxide (NO$_{2}$) and nitrogen monoxide leads to the
formation of ozone (O$_{3}$). This process is the major
photochemical source for ozone in the troposphere concerning
the local as well as the global ozone budget. A new method
for the measurement of atmospheric hydroperoxy and organic
peroxy radical concentrations (HO$_{2}$ and RO$_{2}$) was
developed using the successive conversion of RO$_{2}$ and
HO$_{2}$ to OH radicals which are detected by laser-induced
fluorescence (LIF). The detection system consists of two
differentially pumped chambers. Ambient air is sampled
through a nozzle into the first chamber in which the
pressure is reduced from atmospheric pressure to 25
$\textit{hPa}$. An excess of NO and CO is added downstream
of the inlet, leading to the conversion of RO$_{2}$ to
HO$_{2}$ radicals. The pressure is further reduced in the
second chamber to 3.5 $\textit{hPa}$. HO$_{2}$ is
transformed to OH by the reaction with a further excess of
NO. The detection of OH radicals is achieved by time delayed
gated photon counting after resonant excitation of the
OH-fluorescence at 308$\textit{nm}$ (A$^{2}$Σ$^{+}$ -
X$^{2}$Π). The sensitivity of the system is calibrated
using a radical source in which OH and HO$_{2}$ radicals are
produced by water photolysis. In order to calibrate the
RO$_{2}$ sensitivity, a hydrocarbon is mixed to the
calibration gas. OH reacts quantitatively with the
hydrocarbon resulting in the formation of RO$_{2}$ radicals.
The typical detection limit of the LIF system for peroxy
radicals is 2·10$^{6}$ $\textit{cm}^{−3}$ to 7·10$^{6}$
$\textit{cm}^{−3}$ (0.1 $\textit{pptv}$ to 0.3
$\textit{pptv}$) for an integration time of 30 $\textit{s}$
and for a signal-to-noise-ratio of two. The estimated
accuracy is 10\% which is mainly determined by the
uncertainty of the calibration. Unlike in peroxy radical
amplifier (PERCA) instruments which are used for measuring
HO$_{2}$+RO$_{2}$-radical concentrations, only a weak
dependence of the sensitivity on the water vapor content in
the sampled air is found which can be explained by humidity
dependent quenching of the OH fluorescence. The instrument
was characterized in laboratory measurements. The results
agree with analytic and numerical calculations investigating
the reaction kinetics of the RO$_{2}$ conversion process.
Measurements of peroxy radicals were validated by
simultaneous measurements of the new LIF instrument and an
established measurement technique (Matrix Isolation and
Electron Spin Resonance, MIESR) in experiments at the
atmosphere simulation chamber SAPHIR. The SAPHIR chamber
allows to investigate chemical processes under controlled
atmospheric conditions. First ambient air measurements of
peroxy radicals were performed during the international
field campaign HOxCOMP in July 2005 showing reasonable
diurnal profiles.},
cin = {ICG-II},
ddc = {333.7},
cid = {I:(DE-Juel1)VDB48},
pnm = {Atmosphäre und Klima},
pid = {G:(DE-Juel1)FUEK406},
typ = {PUB:(DE-HGF)11 / PUB:(DE-HGF)3},
url = {https://juser.fz-juelich.de/record/55628},
}