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We describe the physical processes by which a vertically localized absorber perturbs the top-of-atmosphere solar backscattered ultraviolet (UV) radiance. The distinct spectral responses to perturbations of an absorber in its column amount and layer altitude provide the basis for a practical satellite retrieval technique, the Extended Iterative Spectral Fitting (EISF) algorithm, for the simultaneous retrieval of these quantities of a SO2 plume. In addition, the EISF retrieval provides an improved UV aerosol index for quantifying the spectral contrast of apparent scene reflectance at the bottom of atmosphere bounded by the surface and/or cloud; hence it can be used for detection of the presence or absence of UV absorbing aerosols. We study the performance and characterize the uncertainties of the EISF algorithm using synthetic backscattered UV radiances, retrievals from which can be compared with those used in the simulation. Our findings indicate that the presence of aerosols (both absorbing and nonabsorbing) does not cause large errors in EISF retrievals under most observing conditions when they are located below the SO2 plume. The EISF retrievals assuming a homogeneous field of view can provide accurate column amounts for inhomogeneous scenes, but they always underestimate the plume altitudes. The EISF algorithm reduces systematic errors present in existing linear retrieval algorithms that use prescribed SO2 plume heights. Applying the EISF algorithm to Ozone Monitoring Instrument satellite observations of the recent Kasatochi volcanic eruption, we demonstrate the successful retrieval of effective plume altitude of volcanic SO2, and we also show the improvement in accuracy in the corresponding SO2 columns.

[1] The ozone monitoring instrument (OMI), launched on the EOS/Aura satellite in July 2004, makes daily global observations of natural and anthropogenic SO2 emissions with unprecedented spatial resolution. Here we present the first robust comparison of OMI volcanic SO2 retrievals with ground−based instrumentation, using direct Sun observations of the Okmok volcanic cloud from Washington State University (WSU) in Pullman, WA on 18–20 July 2008. These measurements were made by the multifunction differential optical absorption spectroscopy (MFDOAS) instrument developed at WSU, as the Okmok cloud drifted over Pullman in the upper troposphere and lower stratosphere (UTLS). Observation conditions were favorable with cloud-free skies and a relatively homogeneous volcanic cloud distribution on OMI ground pixel scales (∼20–50 km). Movement of the Okmok cloud north and south of Pullman over a period of several days permitted comparison with three OMI overpasses with SO2 column amounts above the SO2 background level. The total SO2 columns measured by MFDOAS during OMI overpasses were 3.11 ± 0.23 Dobson units (DU), 1.75 ± 0.16 DU and 1.22 ± 0.18 DU (1 DU = 2.69 × 1016 molecules/cm2 = 0.029 g/m2). Comparison of ground-based direct Sun and operational and off-line OMI retrievals show an excellent agreement, providing the first validation of OMI measurements of volcanic SO2 in the UTLS.

The development of the springtime (September-November) Antarctic ozone hole was observed by the Meteor 3/total ozone mapping spectromter (TOMS) to result in the lowest ozone value, 85 DU (Dobson units) on October 8, 1993, ever measured by TOMS. During late September and early October the region of extremely low ozone values was centered on the geographical pole between 85 deg S and 90 deg S. The geographical extent of the ozone hole region, the area within the 220-DU contour, reached a maximum during the first week in October at a near-circular area covering 24 x 10(exp 6) sq km reaching to the southern tip of South America. This approximately matched the 1992 area record. After the maximum area was reached in early October, the 1993 ozone hole region was significantly larger than during 1992 throughout the remainder of the month of October. The very low ozone values over the Antarctic continent have been confirmed by independent ground-based data. Unlike 1992, the formation of the 1993 Antarctic ozone hole does not coincide with unusually low ozone values observed over most of the globe for the past 2 years. The most recent ozone data from Meteor 3/TOMS show that there has been a recovery at all latitudes from the extraordinarily low values observed during 1992 and part of 1993 after the June 1991 eruption of Mount Pinatubo. Meteor 3/TOMS is described and compared with Nimbus 7/TOMS during the 1991 to May 1993 overlap period. Observations of the 1992 ozone hole are presented from both instruments and are shown to agree within 5 DU.

The total ozone mapping spectrometer (TOMS), first flown on the Nimbus 7 satellite, has delivered an unanticipated set of unique information about volcanic plumes because of its contiguous spatial mapping and use of UV wavelengths. The accuracies of TOMS sulfur dioxide retrievals, volcanic plume masses, and eruption totals under low-latitude conditions are evaluated using radiative transfer simulations and error analysis. The retrieval algorithm is a simultaneous solution of the absorption optical depth equations including ozone and sulfur dioxide at the four shortest TOMS wavelengths and an empirical correction based on background condition residuals. The retrieval algorithm reproduces model stratospheric sulfur dioxide plume amounts within ±10% over most central scan angles and moderate solar zenith angles if no aerosols or ash are present. The errors grow to 30% under large solar zenith angle conditions. Volcanic ash and sulfate aerosols in the plume in moderate optical depths (0.3) produce an overestimation of the sulfur dioxide by 15–25% depending on particle size and composition. Retrievals of tropospheric volcanic plumes are affected by the reflectivity of the underlying surface or clouds. The precision of individual TOMS SO2 soundings is limited by data quantization to ±6 Dobson units. The accuracy is independent of most instrument calibration errors but depends linearly on relative SO2 absorption cross-section errors at the TOMS wavelengths. Volcanic plume mass estimates are dependent on correction of background offsets integrated over the plume area. The errors vary with plume mass and area, thus are highly individual. In general, they are least for moderate size, compact plumes. Estimates of the total mass of explosively erupted sulfur dioxide depend on extrapolation of a series of daily plume masses backward to the time of the eruption. Errors of 15–30% are not unusual. Effusive eruption total mass estimates are more uncertain due to difficulties in separating new from old sulfur dioxide in daily observations.

Prelaunch and postlaunch calibration results for the Meteor 3/TOMS instrument are presented here. The instrument, launched aboard a Russian spacecraft in 1991, is the second in a series of total ozone mapping spectrometer (TOMS) instruments designed to provide daily global mapping of ozone overburden. Ozone amounts are retrieved from measurements of Earth albedo in the 312- to 380-nm range. The accuracy of albedo measurements is primarily tied to knowledge of the reflective properties of diffusers used in the calibrations and to the instrument's wavelength selection. These and other important prelaunch calibrations are presented. Their estimated accuracies are within the bounds necessary to determine column ozone to better than 1%. However, postlaunch validation results indicate some prelaunch calibration uncertainties may be larger than originally estimated. Instrument calibrations have been maintained postlaunch to within a corresponding 1% error in retrieved ozone. Onboard calibrations, including wavelength monitoring and a three-diffuser solar measurement system, are described and specific results are presented. Other issues, such as the effects of orbital precession on calibration and recent chopper wheel malfunctions, are also discussed.

A mid-latitude northern hemisphere model of the daytime ozone distribution in the troposphere, stratosphere, and lower mesosphere has been constructed. Data from rocket soundings in the latitude range of 45 deg N + or - 15 deg N, results of balloon soundings at latitudes from 41 to 47 deg N, and latitude gradients from satellite ozone observations have been combined to produce estimates of the annual mean ozone concentration and its variability at heights up to 74 km for an effective latitude of 45 deg N. This model is a revision for heights above 26 km of the tentative mid-latitude ozone model, included in the U.S. Standard Atmosphere Supplements, 1966, and has been adopted for use in the U.S. Standard Atmosphere, 1976.

High-energy proton data obtained by polar-orbiting satellite and several balloon flights are used to derive the spatial extent and ionization profiles of regions irradiated by the intense solar particle events (SPE) of August 1972. Backscattered ultraviolet ozone sensors on the Nimbus 4 satellite identified and tracked the polar ozone cavity created by particle ionization during the intense, ten-hour period of August 4, which persisted and rotated as a semirigid mass in an east-to-west direction during 53 days of continuous tracking. Time-dependent chemistry calculations have been performed to show the cause, magnitude, and temporal features of the ozone reduction. Attempts to verify the predicted temperature changes have been unsuccessful due to limitations in the temperature measurement techniques used.

A program designed to study the Antarctic ozone hole using ER-2 high-altitude and DC-8 aircraft was conducted out of Punta Arenas, Chile during August 17-September 22, 1987. Graphs are presented of ozone and chlorine monoxide when crossing the boundary of the chemically perturbed region on August 23 and on September 21. Interpretations of ClO, H2O, and N2O measurements are presented, indicating ongoing diabetic cooling and advective poleward transport across the boundary.

Localized rapid reductions in total ozone (miniholes), which were observed during the Airborne Antarctic Ozone Experiment, are studied with particular attention given to meteorological aspects. It is suggested that miniholes are forced by tropospheric weather features and that they are largely reversible distortions to the airflow around the vortex. The relationship between the miniholes and upper tropospheric and lower stratospheric synoptic-scale disturbances is studied. Trajectory calculations are presented which demonstrate the exchange of air from low latitudes with air from within the vortex, with the vortex air subsequently moving to lower latitudes.

Model simulations were used to investigate the seasonal and interannual behavior of ozone for different choices of initial odd nitrogen concentration in July and different assumptions on the heterogeneous reactions, with particular consideration given to the possible contribution of chlorine chemistry to the ozone hole phenomenon. The numerical experiments were selected based on the simulations of the observed trace gas concentrations during the Airborne Antarctic Ozone Experiment in 1987. In all cases considered, the catalytic cycle associated with the formation and photolysis of Cl2O2 could account for more than half of the photochemical removal of O3 within the Antarctic vortex through mid-September. The reaction of BrO with ClO, which accounts for 15-20 percent of O3 removal in the same period, tends to play a more important role toward the end of September, when the concentration of ClO is expected to decrease. No simple relationship was found between the increase in chlorine lavel and the interannual decrease in Antarctic O3.

Results are presented on ozone measurements in the upper troposphere/lower stratosphere over Antarctica, obtained by NASA DC-8 aircraft during the August/September 1987 Airborne Antarctic Ozone Experiment. The ozone mixing ratios as high as several hundred ppbv were measured, but in all cases these ratios were observed in pockets of upper atmospheric air, both in the vicinity of and away from the location of the ozone hole. The background ozone values in the surrounding troposphere were typically in the range of 20-50 ppbv. Correlation of tropospheric ozone observations with the boundaries of the ozone hole differed in the course of the experiment. During the August 28 - September 2 flights, encounters with ozone-rich air were limited, and the background tropospheric ozone appeared to decrease beneath the hole. For the later flights, and as the ozone hole deepened, the ozone-rich air was frequently observed in the vicinity of the hole, and the average ozone values at the flight altitude were frequently higher than the background values.