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38 CHAPTER 2. ATMOSPHERE AND REMOTE SENSING 2.2.1 Investigation of Inorganic Stratospheric Bromine Participating scientists Dorf, M., A. Butz, F. Weidner, and K. Pfeilsticker Abstract Balloon-borne DOAS (Differential Optical Absorption Spectroscopy) bromine monoxide (BrO) measurements and model simulations are used to investigate the inorganic stratospheric bromine chemistry and to validate BrO limb profiling from the new SCIAMACHY instrument on the European Envisat (ENVIronment SATellite) satellite. Morning Evolution Evening Evolution Time Time Figure 2.14: Colour-coded model concentration field of BrO as a function of height and SZA, for a DOAS balloon flight. Left and right panels show the morning and evening evolution of BrO respectively. The black lines in the left panel represent the line-of-sight of a SCIAMACHY limb scan. In the right panel the observation geometry of the DOAS measurements is shown. The thick black line represents the trajectory of the balloon and the thin black lines indicate the optical path from the Sun to the balloon instrument for measurements during ascent and solar occultation. Background Inorganic bromine (BrY) is the second most important halogen affecting stratospheric ozone. Although much less abundant than chlorine, stratospheric bromine currently contributes about 25 % to global ozone loss. During daylight the most abundant stratospheric bromine species is BrO, which accounts for 60 − 70 % of total BrY and is also the most feasible inorganic bromine species for detection. Balloonborne DOAS BrO measurements are used for validation of the SCIAMACHY satellite instrument. Funding This work was conducted within ESA contracts AO 146 and AO 465. Funding came from the BundesMinisterium <strong>für</strong> Bildung und Forschung (BMBF), contract DLR-50EE0017. Methods and results BrO is subject to considerable diurnal variation. Validation thus requires either perfect collocation of the validation observation with the satellite profiling, or other methods to account properly for temporal or spatial mismatches between both sets of observations and for their different viewing geometry (see figure 2.14). Photochemical modelling along air mass trajectories, which match the balloon with SCIAMACHY observations are used to account for these discrepancies and to generate a BrO profile validation set. First comparisons of SCIA- MACHY limb measurements with high precision DOAS BrO profiles show poor agreement, especially below 20 km, which is presently the most interesting region for bromine chemistry. Outlook/Future work • Investigation of the upper troposphere / lower stratosphere bromine budget • Investigation of the composition of organic bromine source gases • Bromine trend in the stratosphere • Coupling of bromine and chlorine chemistry Main publication Dorf, M., Investigation of Inorganic Stratospheric Bromine using Balloon- Borne DOAS Measurements and Model Simulations, PhD thesis at the University of Heidelberg, Heidelberg, Germany, 2005.
2.2. STRATOSPHERIC OZONE 39 2.2.2 Stratospheric photochemistry of ozone, nitrogen and chlorine species Participating scientists at IUP Heidelberg Butz, A., M. Dorf, F. Weidner, and K. Pfeilsticker Abstract In the recent past the LPMA/DOAS balloon payload has conducted several stratospheric balloon flights at various locations and in different seasons. The inferred abundances of stratospheric ozone (O3) and nitrogen dioxide (NO2) are checked for internal consistency and compared to correlative data measured by the satellite borne instrument SCIAMACHY. Figure 2.15: Relative deviations between satellite (retrieved by IUP Bremen) and balloon borne measurements of O3 (left panel) and NO2 (right panel) vertical profiles. Observation sites and conditions are indicated in the legend. The mean deviation of all coincident data in the 20 km – 31 km altitude is 4.3% with 10.8% standard deviation for O3 and 1.8% with 12.4% standard deviation for NO2. The grey lines indicate the mean and the one and two times standard deviation boundaries with respect to the 20 km – 31 km altitude range. Note the broken abscissa. Background Nitrogen oxides dominate the catalytic destruction of stratospheric O3 between 25 and 40 km altitude. Thus, NO2 and O3 measurements are of primary importance to study stratospheric photochemistry. Recent studies indicate that for selected geophysical conditions the agreement between measured and modeled O3 and NO2 is better than 10%. Accordingly, measurements of high accuracy are required to constrain or to be compared with photochemical models. Our study aims at estimating the accuracy of state-of-the-art remote sensing measurements of O3 and NO2. Funding The present work has been supported by ESA, BMBF, DLR and the European Union. Methods and results Abundances of stratospheric O3 and NO2 inferred from traditional solar occultation measurements of the LPMA/DOAS balloon payload are checked for internal consistency and subsequently compared to collocated observations of the SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY) onboard the European Envisat satellite. Our comparison scheme accounts for the temporal and spatial mismatch (airmass trajectory modell) as well as for the differing photochemical conditions (1D chemistry modell) between the balloon and the satellite borne observations. The internal agreement of the balloon borne measurements is 10% and 20% for O3 and NO2, respectively. Typical deviations between SCIA- MACHY and the balloon borne data amount to 20% for both gases in the 20 to 30 km altitude range, see figure (2.15). Below 20 km the agreement worsens mainly due to lower sensitivity of the satellite retrieval. Outlook/Future work • Extension of the O3 and NO2 validation study to tropical latitudes • Case studies of the stratospheric nitrogen and chlorine budget/partitioning and implications for ozone loss • Abundance of iodine radicals in the tropical upper troposphere and stratosphere Main publication Butz, A. et al., Intercomparison of Stratospheric O3 and NO2 abundances retrieved from balloon borne direct sun observations and Envisat/SCIAMACHY limb measurements, Atmos. Chem. Phys. Disc. 5, 10747– 10797, 2005.
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Institut für Umweltphysik Im Neuen
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