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.

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.

2009, Brovkin, V., Petoukhov, V., Claussen, M., Bauer, E., Archer, D., Jaeger, C.

We use a coupled climate-carbon cycle model of intermediate complexity to investigate scenarios of stratospheric sulfur injections as a measure to compensate for CO2-induced global warming. The baseline scenario includes the burning of 5,000 GtC of fossil fuels. A full compensation of CO2-induced warming requires a load of about 13 MtS in the stratosphere at the peak of atmospheric CO2 concentration. Keeping global warming below 2°C reduces this load to 9 MtS. Compensation of CO 2 forcing by stratospheric aerosols leads to a global reduction in precipitation, warmer winters in the high northern latitudes and cooler summers over northern hemisphere landmasses. The average surface ocean pH decreases by 0.7, reducing the calcifying ability of marine organisms. Because of the millennial persistence of the fossil fuel CO2 in the atmosphere, high levels of stratospheric aerosol loading would have to continue for thousands of years until CO2 was removed from the atmosphere. A termination of stratospheric aerosol loading results in abrupt global warming of up to 5°C within several decades, a vulnerability of the Earth system to technological failure. © 2008 The Author(s).

2008, Sica, R.J., Izawa, M.R.M., Walker, K.A., Boone, C., Petelina, S.V., Argall, P.S., Bernath, P., Burns, G.B., Catoire, V., Collins, R.L., Daffer, W.H., De Clercq, C., Fan, Z.Y., Firanski, B.J., French, W.J.R., Gerard, P., Gerding, M., Granville, J., Innis, J.L., Keckhut, P., Kerzenmacher, T., Klekociuk, A.R., Kyrö, E., Lambert, J.C., Llewellyn, E.J., Manney, G.L., McDermid, I.S., Mizutani, K., Murayama, Y., Piccolo, C., Raspollini, P., Ridolfi, M., Robert, C., Steinbrecht, W., Strawbridge, K.B., Strong, K., Stübi, R., Thurairajah, B.

An ensemble of space-borne and ground-based instruments has been used to evaluate the quality of the version 2.2 temperature retrievals from the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS). The agreement of ACE-FTS temperatures with other sensors is typically better than 2 K in the stratosphere and upper troposphere and 5 K in the lower mesosphere. There is evidence of a systematic high bias (roughly 3–6 K) in the ACE-FTS temperatures in the mesosphere, and a possible systematic low bias (roughly 2 K) in ACE-FTS temperatures near 23 km. Some ACE-FTS temperature profiles exhibit unphysical oscillations, a problem fixed in preliminary comparisons with temperatures derived using the next version of the ACE-FTS retrieval software. Though these relatively large oscillations in temperature can be on the order of 10 K in the mesosphere, retrieved volume mixing ratio profiles typically vary by less than a percent or so. Statistical comparisons suggest these oscillations occur in about 10% of the retrieved profiles. Analysis from a set of coincident lidar measurements suggests that the random error in ACE-FTS version 2.2 temperatures has a lower limit of about ±2 K.

2000, James, P.M., Peters, D., Waugh, D.W.

The large-scale ozone distribution over the northern hemisphere undergoes strong fluctuationseach winter on timescales of up to a few weeks. This is closely linked to changes in the stratosphericpolar vortex, whose shape, intensity and location vary with time. Elliptical diagnosticparameters provide an empirical description of the daily character of the polar vortex. Theseparameters are used as an objective measure to define two characteristic wintertime vortexdisplacements, towards northern Europe and Canada, respectively. The large-scale structuresin both the stratosphere and troposphere and the 3D ozone structures are determined for bothvortex displacement scenarios. A linear ozone transport model shows that the contribution ofhorizontal ozone advection dominates locally in the middle stratosphere. Nevertheless, thelargest contribution is due to vertical advection around the ozone layer maximum. The findingsare in agreement with an EOF analysis which reveals significant general modes of ozone variabilitylinked to polar vortex displacement and to phase-shifted large-scale tropospheric waves.When baroclinic waves travel through the regions of vortex-related ozone reduction, the combinedeffect is to produce transient synoptic-scale areas of exceptionally low ozone; namelydynamically induced strong ozone mini-holes.

2009, Sonnemann, G.R., Hartogh, P.

Ozone measurements taken with a ground based microwave instrument at Lindau (51.66° N, 10.13° E) over some years showed strong ozone decrease events within the stratopause region, particularly during the winter half-year. These events are characterized by a marked drop of the ozone mixing ratio from two to three ppmv to less than half a ppmv in extreme cases. Simultaneous water vapor measurements at the same place, also carried out by a microwave instrument, showed a strong increase of its mixing ratio and the temperature was also enhanced during these episodes. The theoretical analysis brought evidence that these events result from a positive feedback in the complex radiatively-chemical system between the ozone column density and the ozone dissociation rate.