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Satellite-based observations during the Arctic winter of 2009/2010 provide firm evidence that, in contrast to the current understanding, the nucleation of nitric acid trihydrate (NAT) in the polar stratosphere does not only occur on preexisting ice particles. In order to explain the NAT clouds observed over the Arctic in mid-December 2009, a heterogeneous nucleation mechanism is required, occurring via immersion freezing on the surface of solid particles, likely of meteoritic origin. For the first time, a detailed microphysical modelling of this NAT formation pathway has been carried out. Heterogeneous NAT formation was calculated along more than sixty thousand trajectories, ending at Cloud Aerosol Lidar with Orthogonal Polarization (CALIOP) observation points. Comparing the optical properties of the modelled NAT with these observations enabled a thorough validation of a newly developed NAT nucleation parameterisation, which has been built into the Zurich Optical and Microphysical box Model (ZOMM). The parameterisation is based on active site theory, is simple to implement in models and provides substantial advantages over previous approaches which involved a constant rate of NAT nucleation in a given volume of air. It is shown that the new method is capable of reproducing observed polar stratospheric clouds (PSCs) very well, despite the varied conditions experienced by air parcels travelling along the different trajectories. In a companion paper, ZOMM is applied to a later period of the winter, when ice PSCs are also present, and it is shown that the observed PSCs are also represented extremely well under these conditions.

The Gas and Aerosol Measurement Sensor (GAMS) was deployed aboard the NASA DC-8 aircraft during the second SAGE III Ozone Loss and Validation Experiment (SOLVE II). GAMS acquired line-of-sight (LOS) direct solar irradiance spectra during the sunlit portions of ten science flights of the DC-8 between 12 January and 4 February 2003. Differential line-of-sight (DLOS) optical depth spectra are produced from the GAMS raw solar irradiance spectra. Then, DLOS ozone number densities are retrieved from the GAMS spectra using a multiple linear regression spectral fitting technique. Both the DLOS optical depth spectra and retrieved ozone data are compared with coincident measurements from two other solar instruments aboard the DC-8 platform to demonstrate the robustness and stability of the GAMS data. The GAMS ozone measurements are then utilized to evaluate the quality of the Wulf band ozone cross sections, a critical component of the SAGE III aerosol, water vapor, and temperature/pressure retrievals. Results suggest the ozone cross section compilation of Shettle and Anderson currently used operationally in SAGE III data processing may be in error by as much as 10-20% in theWulf bands, and their lack of reported temperature dependence is a significant deficiency. A second, more recent, cross section database compiled for the SCIAMACHY satellite mission appears to be of much better quality in the Wulf bands, but still may have errors as large as 5% near the Wulf band absorption peaks, which is slightly larger than their stated uncertainty. Additional laboratory measurements of the Wulf band cross sections should be pursued to further reduce their uncertainty and better quantify their temperature dependence.

At the beginning of the 1991 Austral spring, volcanic aerosols from Mt. Pinatubo and Cerro Hudson were present in the polar stratosphere of the Southern Hemisphere. Satellite observations of aerosol extinction were used to identify and track the movement of these aerosols in the vicinity of the Antarctic vortex during August through November 1991. A layer of mature Mt. Pinatubo aerosols was identified near 21 km and a layer of fresh Cerro Hudson aerosols was identified near 12 km. This altitude separation of the Mt. Pinatubo and Cerro Hudson aerosols was observed throughout the period. Below 15 km, the polar stratosphere was subject to episodes of strong wave activity which transported the Cerro Hudson aerosols poleward and, after the middle of September, they became a persistent feature beneath the vortex. Above 15 km, signatures of Mt. Pinatubo aerosols were observed near the vortex boundary, but significant portions of the vortex interior remained free of any detectable intrusions of Mt. Pinatubo aerosols until the final warming in mid-November.

A global aerosol climatology is evolving from the NASA satellite experiments SAM II, SAGE I, and SAGE II. In addition, polar stratospheric cloud (PSC) data have been obtained from these experiments over the last decade. An undated reference model of the optical characteristics of the background aerosol is described and a new aerosol reference model derived from the latest available data is proposed. The aerosol models are referenced to the height above the tropopause. The impact of a number of volcanic eruptions is described. In addition, a model describing the seasonal, longitudinal, and interannual variations in PSCs is presented.

The efficiencies of chemical families such as ClO(x) and NO(x) for altering the total abundance and distribution of stratospheric ozone are controlled by a partitioning between reactive (active) and nonreactive (reservoir) compounds within each family. Gas phase thermodynamics, photochemistry, and kinetics would dictate, for example, that only about 1 percent of the chlorine resident in the lower stratosphere would be in the form of active Cl or ClO, the remainder existing in the reservoir compounds HCl and ClONO2. The consistency of this picture was recently challenged by the recognition that important chemical transformations take place on polar regions: the Airborne Antarctic Ozone Experiment (AAOE) and the Airborne Arctic Stratospheric Expedition (AASA). Following the discovery of the Antarctic ozone hole, Solomon et al. suggested that the heterogeneous chemical reaction: ClONO2(g)+HCl(s) yields Cl2(g)+HNO3(s) could play a key role in converting chlorine from inactive forms into a species (Cl2) that would rapidly dissociate in sunlight to liberate atomic chlorine and initiate ozone depletion. The symbols (s) and (g) denote solid phase, or adsorbed onto a solid surface, and gas phase, respectively, and represent the approach by which such a reaction is modeled rather than the microscopic details of the reaction. The reaction was expected to be most important at altitudes where PSC's were most prevalent (10 to 25 km), thereby extending the altitude range over which chlorine compounds can efficiently destroy ozone from the 35 to 45 km region (where concentrations of active chlorine are usually highest) to lower altitudes where the ozone concentration is at its peak. This chapter will briefly review the current state of knowledge of heterogeneous processes in the stratosphere, emphasizing those results obtained since the World Meteorological Organization (WMO) conference. Sections are included on laboratory investigations of heterogeneous reactions, the characteristics and climatology of PSC's, stratospheric sulfate aerosols, and evidence of heterogeneous chemical processing.

Polar stratospheric clouds (PSCs) form at very cold temperatures which typically occur only at high latitudes during local winter. However, meteorological circumstances in the Arctic during late January 1989 led to PSC formation unusually far to the south, at latitudes (near 50 deg N) being sampled during the period by the orbiting SAGE II instrument. These unusual PSC sightings and the evolution of meteorological conditions which produced the episode are described. Profiles of SAGE II extinction measurements at 0.525 and 1.02 microns show clear signatures of PSCs and indicate that the cloud particles were considerably larger than the background aerosol. It is most important to note that the clouds were sighted at a latitude where there was extensive sunlight, thus increasing the likelihood of ozone loss both locally and downstream due to enhancements in reactive chlorine expected from heterogeneous chemical processing within the PSCs.

The Stratospheric Aerosol Measurement II (SAM II) satellite experiment measures 14 daily 1.0-micron aerosol extinction profiles in the high northern latitudes. These SAM II data were used to spot the locations of polar stratospheric clouds (PSCs) and provide an overview of the vertical structure of the upper tropospheric and stratospheric aerosols during the 1989 Airborne Arctic Stratospheric Expedition (AASE). Although SAM II measured a higher than average number of PSCs in January 1989 as compared to the previous 10 years, the number of PSCs sighted during the entire 1989 winter season is only slightly above average. Also discussed is the vertical gradient in aerosol extinction which occurs as the SAM II measurement locations cross the polar vortex.

Data on monthly latitudinal variations in middle-atmosphere vertical ozone profiles are presented, based on extensive Nimbus-7, AE-2, and SME satellite measurements from the period 1978-1982. The coverage of the data sets, the characteristics of the sensors, and the analysis techniques applied are described, and the results are compiled in tables and graphs. These ozone data are intended to supplement the models of the 1986 COSPAR International Reference Atmosphere.

This paper describes the improvements introduced into the original version of ozone reference model of Keating and Young (1985, 1987) which is to be incorporated in the next COSPAR International Reference Atmosphere (CIRA). The ozone reference model will provide information on the global ozone distribution (including the ozone vertical structure as a function of month and latitude from 25 to 90 km) combining data from five recent satellite experiments: the Nimbus 7 LIMS, Nimbus 7 SBUV, AE-2 Stratospheric Aerosol Gas Experiment (SAGE), Solar Mesosphere Explorer (SME) UV Spectrometer, and SME 1.27 Micron Airglow. The improved version of the reference model uses reprocessed AE-2 SAGE data (sunset) and extends the use of SAGE data from 1981 to the 1981-1983 time period. Comparisons are presented between the results of this ozone model and various nonsatellite measurements at different levels in the middle atmosphere.

Improvements are provided for the ozone reference model which is to be incorporated in the COSPAR International Reference Atmosphere (CIRA). The ozone reference model will provide considerable information on the global ozone distribution, including ozone vertical structure as a function of month and latitude from approximately 25 to 90 km, combining data from five recent satellite experiments (Nimbus 7 LIMS, Nimbus 7 SBUV, AE-2 SAGE, Solar Mesosphere Explorer (SME) UVS, and SME IR). The improved models are described and use reprocessed AE-2 SAGE data (sunset) and extend the use of SAGE data from 1981 to the period 1981-1983. Comparisons are shown between the ozone reference model and various nonsatellite measurements at different levels in the middle atmosphere.

Models of ozone vertical structure were generated that were based on multiple data sets from satellites. The very good absolute accuracy of the individual data sets allowed the data to be directly combined to generate these models. The data used for generation of these models are from some of the most recent satellite measurements over the period 1978 to 1983. A discussion is provided of validation and error analyses of these data sets. Also, inconsistencies in data sets brought about by temporal variations or other factors are indicated. The models cover the pressure range from from 20 to 0.003 mb (25 to 90 km). The models for pressures less than 0.5 mb represent only the day side and are only provisional since there was limited longitudinal coverage at these levels. The models start near 25 km in accord with previous COSPAR international reference atmosphere (CIRA) models. Models are also provided of ozone mixing ratio as a function of height. The monthly standard deviation and interannual variations relative to zonal means are also provided. In addition to the models of monthly latitudinal variations in vertical structure based on satellite measurements, monthly models of total column ozone and its characteristic variability as a function of latitude based on four years of Nimbus 7 measurements, models of the relationship between vertical structure and total column ozone, and a midlatitude annual mean model are incorporated in this set of ozone reference atmospheres. Various systematic variations are discussed including the annual, semiannual, and quasibiennial oscillations, and diurnal, longitudinal, and response to solar activity variations.

Observations of Antarctic polar stratospheric clouds (PSCs) were examined using the 1-micron aerosol extinction ratio data from the SAM II satellite experiment for the years 1979-1982 and 1984-1987. PSCs were sighted between 10 and 25 km and were usually first observed by mid-June. Clouds disappeared earlier at higher altitudes (late August near 24 km, in most cases) and later at lower altitudes (late September or October near 16 km). It was found that PSCs persisted longer in 1985 and 1987 at 18 km and were more frequently observed in September and October 1987 than the other years. Inference of likely PSC formation regions from National Meteorological Center temperature data indicated that clouds would begin forming in late May and usually disappear in September. This analysis confirmed the persistence of colder conditions during the spring of 1987.

The Dynamics Explorer (DE) satellite carries an Auroral Imaging Package which contains filters designed for performing backscatter ultraviolet measurements to measure total column ozone in the Earth's middle and lower atmosphere. Measurements are obtained at 317.5 mm (to measure ozone absorption) and 360 nm (to measure scene reflectivity). In October 1985 and 1986, measurements were obtained near apogee of the Antarctic ozone hole. The only other high spatial resolution measurements were obtained from the Nimbus 7 Total Ozone Mapping Spectrometer (TOMS) experiment. In October 1987, the Dynamics Explorer apogee had precessed into the Northern Hemisphere preventing measurements of the ozone hole. However, measurements should be obtained from DE of the ozone hole in both 1988 and 1989. Considering that the Nimbus 7 TOMS instrument has long exceeded its expected lifetime, the DE Spin Scan Ozone Imager (SOI) experiment could easily play a crucial role in studies of the ozone hole over the next few years.

The data bases and computational techniques used in recent models of the O3 distribution in the earth atmosphere are described, summarizing the results of ongoing efforts to define an O3 reference model for incorporation into CIRA. Consideration is given to the analysis of data from satellite instruments (Nimbus 7 LIMS, TOMS, and SBUV; SME UVS and IR; and AE-2 SAGE) to construct models of total column O3 and vertical O3 structure. The satellite-based model predictions are then compared with balloon, rocket, and umkehr measurements in extensive graphs: good agreement is demonstrated both among the satellite data sets and between satellite and nonsatellite data sets.

Ozone reference models are proposed here similar to the Keating and Young (1985) models which were prepared for the new COSPAR International Reference Atmosphere. This paper updates tables provided in the Keating and Young ozone model, giving improved monthly zonal mean total column ozone in 10 deg latitude increments, improved monthly zonal mean ozone volume mixing ratios (ppmv) from 20 to 0.003 mb in 10 deg latitude increments, and conversion tables providing ozone vertical structure in other units. Also, a new table is provided giving ozone vertical structure as a function of altitude (from 25 to 80 km), latitude, and month. The models are based on measurements from six contemporary satellite instruments.

The effects of solar UV variability on ozone and temperature are studied using Nimbus 7 stratospheric and mesospheric ozone, temperature, and 205-nm solar UV data, and Solar Mesosphere Explorer 1.27-micron ozone and 121.6-nm solar UV data. Consideration is given to the temperature/UV relation, the O3/UV relation with and without temperature feedback, and the responses of HNO3 and NO2 to solar UV variability. It is observed that the response times of temperature to solar UV variability are 6 days at 2 mbar and 1 day at 0.01 mbar. The stratospheric ozone response (with no correction for temperature effects) increases, while in the mesosphere a decrease is detected. The responses of ozone and temperature to solar variability are examined and calculated using a one-dimensional chemical-radiative time-dependent model. The comparison of the model results with the satellite-observed responses reveals generally good correlation between the data; however, the model predicts a larger time lag of the temperature response and a larger stratospheric HNO3 mixing ratio than the satellite data. It is noted that the relation between short-term variations in the solar UV radiation and stratospheric ozone is affected by the coupling between ozone and temperature.

Thirty-eight latitudinal cross sections of stratospheric ozone observed by the SAGE (Stratospheric Aerosol and Gas Experiment) and SBUV (Solar Backscattered Ultraviolet) satellite instruments on the same days in March and April 1979 and at approximately the same latitude are compared. Differences in the zonal-mean mixing ratios are found. At pressures less than 5 mbar, SAGE gives approximately 20 percent larger mixing ratios at tropical latitudes (after a correction has been applied for the expected diurnal variation of ozone). The uncorrelated portion of the SBUV variances are smaller than the SAGE noise variances at altitudes above 10 mbar, which indicates that the SBUV experiment should provide excellent detectability of longitudinal ozone variations.