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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 />

1<br />

-1

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