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2.2. STRATOSPHERIC RESEARCH GROUP 43<br />
2.2.5 Photolytic lifetime of stratospheric N2O5<br />
Lena Kritten (André Butz, Marcel Dorf, Sebastian Kreycy, Cristina Prados, Ulrike Reichl, Benjamin<br />
Simmes, Frank Weidner, Klaus Pfeilsticker)<br />
Abstract Time-dependent profiles of atmospheric radicals were measured in the upper troposphere<br />
and stratosphere during the first international high-altitude balloon campaign in the tropics (Teresina,<br />
Brazil, 5.1 ◦ S, 42.9 ◦ W). The observed diurnal variation of stratospheric NO2 [Weidner et al. , 2005]<br />
in conjunction with photochemical modelling allows to infer the photolytic lifetime of N2O5.<br />
Altitude / km<br />
30<br />
25<br />
20<br />
15<br />
11 12 13 14 15 16<br />
T ime / UT<br />
11 12 13 14 15 16<br />
T ime / UT<br />
[10<br />
17<br />
8 molec/cm 3 ]<br />
Figure 2.21: Measured (left side) and modelled (right side) concentration of NO2 inferred from DOAS<br />
scanning limb observations on the LPMA/IASI payload on June 30, 2005.<br />
Background The amount and partitioning of<br />
stratospheric NOx (NO, NO2 and NO3) and NOy<br />
(NOx, N2O5, HNO3, ClONO2, HO2NO2, and<br />
BrONO2) largely govern ozone photochemistry<br />
in the mid-stratosphere (25-40 km). During daytime,<br />
the tropical NOx is mainly supplied by the<br />
photochemical decay of the nighttime reservoir<br />
N2O5. Monitoring the diurnal variation of NO2<br />
thus provides information on the photolytic lifetime<br />
of N2O5.<br />
Methods and results Within the framework<br />
of an international measurement campaign dedicated<br />
to the ENVISAT/SCIAMACHY validation,<br />
three stratospheric balloon flights of the<br />
mini-DOAS scanning limb instrument were performed<br />
aboard the MIPAS-B, LPMA/DOAS and<br />
IASI balloon payloads in tropical latitudes near<br />
Teresina, Northern Brazil. During all flights the<br />
UV/Vis spectrometer recorded spectra of sunlight<br />
scattered near the horizon in the atmosphere.<br />
Scanning elevation angles range between 0 ◦ and<br />
−6 ◦ with the balloons floating around 33 km altitude.<br />
The spectral retrieval of the obtained skylight<br />
spectra relies on the DOAS method. Pro-<br />
NO 2<br />
file information is then obtained using established<br />
inversion techniques (optimal estimation<br />
technique) in combination with a 3-D radiative<br />
transfer model [Weidner et al. , 2005]. The obtained<br />
profiles of O3 and NO2 are compared to<br />
the outputs of a 1-D photochemical model, which<br />
was initialized with trace gas observations of the<br />
LPMA/DOAS and MIPAS payloads. From the<br />
observed increase of stratospheric NO2 at daytime,<br />
current estimates for the photolysis frequency<br />
of N2O5 can be tested.<br />
Outlook/Future work<br />
Check the photolytic lifetime of N2O5.<br />
Analysis of all three balloon flights at Teresina for<br />
UV/Vis absorbing gases such as O3, NO2, BrO,<br />
OClO, IO, OIO, and CH2O.<br />
Preparation of, and participation in, future measurement<br />
campaigns (at Kiruna in April 2007 and<br />
at Teresina in Sept. 2007).<br />
Funding comes through ESA, BMBF, DFG,<br />
and the European Union.<br />
15<br />
13<br />
11<br />
9<br />
7<br />
5<br />
3<br />
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