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End date: 2009 × Start date: 2000 × Has files: Yes × Type: Text × Publisher: Göttingen : Copernicus GmbH × Subject: atmospheric chemistry ×

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    Sensitivity of polar stratospheric ozone loss to uncertainties in chemical reaction kinetics
    (Göttingen : Copernicus GmbH, 2009) Kawa, S.R.; Stolarski, R.S.; Newman, P.A.; Douglass, A.R.; Rex, M.; Hofmann, D.J.; Santee, M.L.; Frieler, K.
    The impact and significance of uncertainties in model calculations of stratospheric ozone loss resulting from known uncertainty in chemical kinetics parameters is evaluated in trajectory chemistry simulations for the Antarctic and Arctic polar vortices. The uncertainty in modeled ozone loss is derived from Monte Carlo scenario simulations varying the kinetic (reaction and photolysis rate) parameters within their estimated uncertainty bounds. Simulations of a typical winter/spring Antarctic vortex scenario and Match scenarios in the Arctic produce large uncertainty in ozone loss rates and integrated seasonal loss. The simulations clearly indicate that the dominant source of model uncertainty in polar ozone loss is uncertainty in the Cl2O 2 photolysis reaction, which arises from uncertainty in laboratory-measured molecular cross sections at atmospherically important wavelengths. This estimated uncertainty in JCl 2O2 from laboratory measurements seriously hinders our ability to model polar ozone loss within useful quantitative error limits. Atmospheric observations, however, suggest that the Cl2O2 photolysis uncertainty may be less than that derived from the lab data. Comparisons to Match, South Pole ozonesonde, and Aura Microwave Limb Sounder (MLS) data all show that the nominal recommended rate simulations agree with data within uncertainties when the Cl2O2 photolysis error is reduced by a factor of two, in line with previous in situ ClOx measurements. Comparisons to simulations using recent cross sections from Pope et al. (2007) are outside the constrained error bounds in each case. Other reactions producing significant sensitivity in polar ozone loss include BrO + ClO and its branching ratios. These uncertainties challenge our confidence in modeling polar ozone depletion and projecting future changes in response to changing halogen emissions and climate. Further laboratory, theoretical, and possibly atmospheric studies are needed.
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    On the two-day oscillations and the day-to-day variability in global 3-D-modeling of the chemical system of the upper mesosphere/mesopause region
    (Göttingen : Copernicus GmbH, 2005) Sonnemann, G.R.; Grygalashvyly, M.
    The integration of the photochemical system of the upper mesosphere/ mesopause region brought evidence that the system is able to respond in a nonlinear manner under certain conditions. Under the action of the diurnallyperiodic insolation, the system creates subharmonic oscillations or chaos if disregarding strong diffusion, and under special conditions it possesses multiple solutions. The models used in the past were simplified and idealized in view of the number of dimensions and the consideration of the full dynamics. On the basis of our global 3-D-model of the dynamics and chemistry of the middle atmosphere (COMMAIAP), we also found a nonlinear response in the photochemistry under realistic conditions. The model under consideration is not yet self-consistent, but the chemical model uses the dynamical fields calculated by the dynamic model. From our calculations we got period-2 oscillations of the photochemical system within confined latitudinal regions around the solstices but not during the equinoxes. The consequence of the period-2 oscillation of the chemical active minor constituents is that a marked two-day variation of the chemical heating rates is an important thermal pumping mechanism. We discuss these findings particularly in terms of the influence of realistic dynamics on the creation of nonlinear effects.