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Sensitivity of polar stratospheric ozone loss to uncertainties in chemical reaction kinetics

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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Longitude-dependent decadal ozone changes and ozone trends in boreal winter months during 1960-2000

2008, Peters, D.H.W., Gabriel, A., Entzian, G.

This study examines the longitude-dependent decadal changes and trends of ozone for the boreal winter months during the period of 1960–2000. These changes are caused primarily by changes in the planetary wave structure in the upper troposphere and lower stratosphere. The decadal changes and trends over 4 decades of geopotential perturbations, defined as a deviation from the zonal mean, are estimated by linear regression with time. The decadal changes in longitude-dependent ozone were calculated with a simple transport model of ozone based on the known planetary wave structure changes and prescribed zonal mean ozone gradients. For December of the 1960s and 1980s a statistically significant Rossby wave track appeared over the North Atlantic and Europe with an anticyclonic disturbance over the Eastern North Atlantic and Western Europe, flanked by cyclonic disturbances. In the 1970s and 1990s statistically significant cyclonic disturbances appeared over the Eastern North Atlantic and Europe, surrounded by anticyclonic anomalies over Northern Africa, Central Asia and Greenland. Similar patterns have been found for January. The Rossby wave track over the North Atlantic and Europe is stronger in the 1980s than in the 1960s. For February, the variability of the regression patterns is higher. For January we found a strong alteration in the modelled decadal changes in total ozone over Central and Northern Europe, showing a decrease of about 15 DU in the 1960s and 1980s and an increase of about 10 DU in the 1970s and 1990s. Over Central Europe the positive geopotential height trend (increase of 2.3 m/yr) over 40 years is of the same order (about 100 m) as the increase in the 1980s alone. This is important to recognize because it implies a total ozone decrease over Europe of the order of 14 DU for the 1960–2000 period, for January, if we use the standard change regression relation that about a 10-m geopotential height increase at 300 hPa is related to about a 1.4-DU total ozone decrease.