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Cunnold, D.

Publications and source records attributed to Cunnold, D..

Temporal Decrease in Upper Atmospheric Chlorine

We report a steady decrease in the upper stratospheric and lower mesospheric abundances of hydrogen chloride (HCl) from August 2004 through January 2006, as measured by the Microwave Limb Sounder (MLS) aboard the Aura satellite. For 60(deg)S to 60(deg)N zonal means, the average yearly change in the 0.7 to 0.1 hPa (approx.50 to 65 km) region is -27 +/- 3 pptv/year, or -0.78 +/- 0.08 percent/year. This is consistent with surface abundance decrease rates (about 6 to 7 years earlier) in chlorine source gases. The MLS data confirm that international agreements to reduce global emissions of ozone-depleting industrial gases are leading to global decreases in the total gaseous chlorine burden. Tracking stratospheric HCl variations on a seasonal basis is now possible with MLS data. Inferred stratospheric total chlorine (CITOT) has a value of 3.60 ppbv at the beginning of 2006, with a (2-sigma) accuracy estimate of 7%; the stratospheric chlorine loading has decreased by about 43 pptv in the 18-month period studied here. We discuss the MLS HCl measurements in the context of other satellite-based HCl data, as well as expectations from surface chlorine data. A mean age of air of approx. 5.5 years and an age spectrum width of 2 years or less provide a fairly good fit to the ensemble of measurements.

chlorine

Global average concentration and trend for hydroxyl radicals deduced from ALE/GAGE trichloroethane (methyl chloroform) data for 1978-1990

An optimal estimation inversion scheme is utilized with atmospheric data and emission estimates to determined the globally averaged CH3CCl3 tropospheric lifetime and OH concentration. The data are taken from atmospheric measurements from surface stations of 1,1,1-trichloroethane and show an annual increase of 4.4 +/- 0.2 percent. Industrial emission estimates and a small oceanic loss rate are included, and the OH concentration for the same period (1978-1990) are incorporated at 1.0 +/- 0.8 percent/yr. The positive OH trend is consistent with theories regarding OH and ozone trends with respect to land use and global warming. Attention is given to the effects of the ENSO on the CH3CCl3 data and the assumption of continuing current industrial anthropogenic emissions. A novel tropical atmospheric tracer-transport mechanism is noted with respect to the CH3CCl3 data.

Prinn, R.

Atmospheric emissions and trends of nitrous oxide deduced from 10 years of ALE-GAGE data

Long-term measurements of nitrous oxide (N2O) obtained during the Atmospheric Lifetime Experiment (ALE) and the Global Atmospheric Gases Experiment (GAGE) for a period from 1978 to 1988 are presented and interpreted. It is observed that the average concentration in the Northern Hemisphere is 0.75 +/- 0.16 ppbv higher than in the Southern Hemisphere and that the global average linear trend in N2O lies in the range from 0.25 to 0.31 percent/year. The measured trends and latitudinal distributions are shown to be consistent with the hypothesis that stratospheric photodissociation is the major atmospheric sink for N2O, while the cause of the N2O trend is suggested to be a combination of a growing tropical source and a growing Northern mid-latitude source. A 10-year average global N2O emission rate of (20.5 +/- 2.4) x 10 to the 12th g N2O/year is deduced from the ALE/GAGE data.

Prinn, R.

Trends in ozone profile measurements

From an examination of the agreements and differences between different satellite instruments, it is difficult to believe that existing satellite instruments determine upper stratospheric ozone much better than 4 pct.; by extension, it probably would require at least a 4 pct. change to be reliably detected as a change. The best estimates of the vertical profiles of ozone change in the upper stratosphere between 1979 and 1986 are judged to be those given by the two SAGE satellite instruments. SAGE-2 minus SAGE-1 gives a much lower ozone reduction than that given by the archived Solar Backscatter UV data. The average SAGE profiles of ozone changes between 20 and 50 degs north and between 20 and 50 degs south are given. The SAGE-1 and SAGE-2 comparison gives an ozone reduction of about 4 pct. at 25 km over temperate latitudes. Five ground based Umkehr stations between 36 and 52 degs north, corrected for the effects of volcanic aerosols, report an ozone reduction between 1979 and 1987 at Umkehr layer 8 of 9 + or - 5 pct. The central estimate of upper stratospheric ozone reduction given by SAGE at 40 km is less than the central value estimated by the Umkehr method at layer 8.

Johnston, H.

Atmospheric trends in methylchloroform and the global average for the hydroxyl radical

ALE-GAGE (Atmospheric Lifetime Experiment-Global Atmospheric Gases Experiment) data obtained over the seven-year period from July 1978 to June 1985 are presented and interpreted. The data, combined with knowledge of industrial emissions, are used in an optimal estimation inversion scheme to deduce a globally average methylchloroform atmospheric lifetime of 6.3(+ 1.2, - 0.9) years (1 sigma uncertainty) and a globally averaged tropospheric hydroxyl radical concentration of (7.7 + or - 1.4) x 10 to the 5th radicals/cu cm (1 sigma uncertainty). These results provide the most accurate estimates yet of the trends and lifetime of methylchloroform and of the global average for tropospheric hydroxyl radical levels.

Prinn, R.

Comparison of ozone data derived from SBUV and SAGE with emphasis on longitudinal variations

Stratospheric ozone observations performed by the SBAV and SAGE satellite instruments in March and April 1979 are analyzed and compared to other data, where available; in the absence of ground-truth data the experimental uncertainties are modeled by intercomparison of the measurements. The signal-to-noise ratios for the detectability of longitudinal variation in ozone are estimated for both SBUV and SAGE instruments. The analysis of longitudinal variation data reveals significant differences in amplitudes obtained in individual events in which rapid amplitude changes with height were present. Finally, a systematic overestimation of ozone by 20 percent by the SAGE instrument and underestimation by SBUV by about 15 percent at 50-70 latitudes at 10 mb is noted.

Cunnold, D.

A three-dimensional dynamical-chemical model of atmospheric ozone

A three-year integration of a global three-dimensional model including dynamics and simple photochemistry is used to predict ozone. Good agreement with observation is obtained for stratospheric motion patterns, meridional circulations, ozone density as a function of height and latitude, eddy transports of ozone, surface destruction of ozone, and correlations of ozone with other variables. The annual cycle of columnar ozone in high latitudes is present, but at a smaller amplitude than observed. Vertical transport of ozone downward from the main generation level at 30 km is accomplished primarily by small-scale eddy diffusion between 20 and 30 km and again near the ground; large-scale vertical transport dominates in between. The model predicts a secondary maximum in ozone mixing ratio at 45 km somewhat equatorward of the winter polar-night zone. This feature, recently observed from satellite measurements, is thought to be caused by the temperature dependence of reaction rates in the Chapman scheme. The principal deficiency of the model is an underprediction of the spring ozone concentration in high latitudes in the lower stratosphere.

Cunnold, D.