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High mixing ratios of ozone (O3) in the northern Front Range (NFR) of Colorado are not limited to the urban Denver area but were also observed in rural areas where oil and gas activity is the primary source of O3 precursors. On individual days, oil and gas O3 precursors can contribute in excess of 30 ppb to O3 growth and can lead to exceedances of the EPA O3 National Ambient Air Quality Standard. Data used in this study were gathered from continuous surface O3 monitors for June-August 2013-2015 as well as additional flask measurements and mobile laboratories that were part of the FRAPPE/DISCOVER-AQ field campaign of July-August 2014. Overall observed O3 levels during the summer of 2014 were lower than in 2013, likely due to cooler and damper weather than an average summer. This study determined the median hourly surface O3 mixing ratio in the NFR on summer days with limited photochemical production to be approximately 45-55 ppb. Mobile laboratory and flask data collected on three days provide representative case studies of different O3 formation environments in and around Greeley, Colorado. Observations of several gases (including methane, ethane, CO, nitrous oxide) along with O3 are used to identify sources of O3 precursor emissions. A July 23 survey demonstrated low O3 (45-60 ppb) while August 3 and August 13 surveys recorded O3 levels of 75-80 ppb or more. August 3 exemplifies influence of moderate urban and high oil and gas O3 precursor emissions. August 13 demonstrates high oil and gas emissions, low agricultural emissions, and CO measurements that were well correlated with ethane from oil and gas, suggesting an oil and gas related activity as a NOx and O3 precursor source. Low isoprene levels indicated that they were not a significant contributor to O3 precursors measured during the case studies.

Tropospheric ozone plays a major role in Earth's atmospheric chemistry processes and also acts as an air pollutant and greenhouse gas. Due to its short lifetime, and dependence on sunlight and precursor emissions from natural and anthropogenic sources, tropospheric ozone's abundance is highly variable in space and time on seasonal, interannual and decadal time-scales. Recent, and sometimes rapid, changes in observed ozone mixing ratios and ozone precursor emissions inspired us to produce this up-to-date overview of tropospheric ozone's global distribution and trends. Much of the text is a synthesis of in situ and remotely sensed ozone observations reported in the peer-reviewed literature, but we also include some new and extended analyses using well-known and referenced datasets to draw connections between ozone trends and distributions in different regions of the world. In addition, we provide a brief evaluation of the accuracy of rural or remote surface ozone trends calculated by three state-of-the-science chemistry-climate models, the tools used by scientists to fill the gaps in our knowledge of global tropospheric ozone distribution and trends.

We investigated water vapor variations in the tropical lower stratosphere on seasonal, quasi-biennial oscillation (QBO), and decadal time scales using balloon-borne cryogenic frost point hygrometer data taken between 1993 and 2009 during various campaigns including the Central Equatorial Pacific Experiment (March 1993), campaigns once or twice annually during the Soundings of Ozone and Water in the Equatorial Region (SOWER) project in the eastern Pacific (1998-2003) and in the western Pacific and Southeast Asia (2001-2009), and the Ticosonde campaigns and regular sounding at Costa Rica (2005-2009). Quasi-regular sounding data taken at Costa Rica clearly show the tape recorder signal. The observed ascent rates agree well with the ones from the Halogen Occultation Experiment (HALOE) satellite sensor. Average profiles from the recent five SOWER campaigns in the equatorial western, Pacific in northern winter and from the three Ticosonde campaigns at Costa Rica (10degN) in northern summer clearly show two effects of the QBO. One is the vertical displacement of water vapor profiles associated with the QBO meridional circulation anomalies, and the other is the concentration variations associated with the QBO tropopause temperature variations. Time series of cryogenic frost point hygrometer data averaged in a lower stratospheric layer together with HALOE and Aura Microwave Limb Sounder data show the existence of decadal variations: The mixing ratios were higher and increasing in the 1990s, lower in the early 2000s, and probably slightly higher again or recovering after 2004. Thus linear trend analysis is not appropriate to investigate the behavior of the tropical lower stratospheric water vapor.

We present comparisons of observed tropical and sub-tropical ozone from the Southern Hemisphere Additional Ozonesondes (SHADOZ) project with satellite measurements using Aura's Ozone Monitoring Instrument (OMI) and Microwave Limb Sounder (MLS) instruments. Satellite products of total and derived tropospheric column ozone from OMI and profiles of ozone in the UT/LS region from MLS are used.

A solar occultation sensor, the Improved Limb Atmospheric Spectrometer (ILAS)-II, measured 5890 vertical profiles of ozone concentrations in the stratosphere and lower mesosphere and of other species from January to October 2003. The measurement latitude coverage was 54-71degN and 64-88degS, which is similar to the coverage of ILAS (November 1996 to June 1997). One purpose of the ILAS-II measurements was to continue such high-latitude measurements of ozone and its related chemical species in order to help accurately determine their trends. The present paper assesses the quality of ozone data in the version 1.4 retrieval algorithm, through comparisons with results obtained from comprehensive ozonesonde measurements and four satellite-borne solar occultation sensors. In the Northern Hemisphere (NH), the ILAS-II ozone data agree with the other data within +/-10% (in terms of the absolute difference divided by its mean value) at altitudes between 11 and 40 km, with the median coincident ILAS-II profiles being systematically up to 10% higher below 20 km and up to 10% lower between 21 and 40 km after screening possible suspicious retrievals. Above 41 km, the negative bias between the NH ILAS-II ozone data and the other data increases with increasing altitude and reaches 30% at 61-65 km. In the Southern Hemisphere, the ILAS-II ozone data agree with the other data within 10% in the altitude range of 11-60 km, with the median coincident profiles being on average up to 10% higher below 20 km and up to 10% lower above 20 km.

The SHADOZ (Southern Hemisphere Additional Ozonesondes) ozone sounding network was initiated in 1998 to improve the coverage of tropical in-situ ozone measurements for satellite validation, algorithm development and related process studies. Over 2000 soundings have been archived at the website, http://croc.gsfc.nasa.gov/shadoz, for 12 stations: Ascension Island; Nairobi and Malindi, Kenya; Irene, South Africa; Reunion Island; Watukosek, Java; Fiji; Tahiti; American Samoa; San Cristobal, Galapagos; Natal, Brazil; Paramaribo, Surinam. Key results from SHADOZ will be described from among the following: 1) By using ECC sondes with similar procedures, 5-10% accuracy and precision (1-sigma) of the sonde total ozone measurement is achieved; 2) Week-to-week variability in tropospheric ozone is so great that statistics are frequently not Gaussian; most stations vary up to a factor of 3 in tropospheric column over the course of a year; 3) Longitudinal variability in tropospheric ozone profiles is a consistent feature, with a 10-15 DU column-integrated difference between Atlantic and Pacific sites; this causes a "zonal wave-one" feature in total ozone; 4) The ozone record from Paramaribo, Surinam (6N, 55W) is a marked contrast to southern tropical ozone because Surinam is often north of the Intertropical Convergence Zone.

Ozone profile data from soundings integrate models, aircraft and other ground-based measurements for better interpretation of atmospheric chemistry and dynamics. A well-designed network of ozonesonde stations, with consistent sampling, can answer questions not possible with short campaigns or current satellite technology. The SHADOZ (Southern Hemisphere Additional Ozonesondes) project, for example, has led to these findings about tropical ozone: definition of the zonal tropospheric wave-one pattern in equatorial ozone, characterization of the "Atlantic ozone paradox" and establishment of a link between tropical Atlantic and Indian Ocean pollution. Building on the SHADOZ concept, a short-term ozone network was formed in July-August 2004 to coordinate ozonesonde launches during the ICARTT/INTEX/NEAQS (International Consortium on Atmospheric Research on Transport and Transformation)/Intercontinental Transport Experiment/New England Air Quality Study. In IONS (INTEX Ozonesonde Network Study), more than 250 soundings, with daily frequency at half the sites, were launched from eleven North American stations and an oceanographic ship in the Gulf of Maine. Although the goal was to examine pollution influences under stable high-pressure systems and transport associated with "warm conveyor belt" flows, the INTEX study region was dominated by a series of weak frontal system that mixed aged pollution with stratospheric ozone in the middle troposphere. Deconvoluting ozone sources provides new insights into ozone in the transition between mid-latitude and polar air.

Since 1998 the Southern Hemisphere ADditional OZonesondes (SHADOZ) project has provided over 2000 ozone profiles over eleven southern hemisphere tropical and subtropical stations. Balloon-borne electrochemical concentration cell (ECC) ozonesondes are used to measure ozone. The data are archived at: &ttp://croc.gsfc.nasa.gov/shadoz>. In analysis of ozonesonde imprecision within the SHADOZ dataset, Thompson et al. [JGR, 108,8238,20031 we pointed out that variations in ozonesonde technique (sensor solution strength, instrument manufacturer, data processing) could lead to station-to-station biases within the SHADOZ dataset. Imprecisions and accuracy in the SHADOZ dataset are examined in light of new data. First, SHADOZ total ozone column amounts are compared to version 8 TOMS (2004 release). As for TOMS version 7, satellite total ozone is usually higher than the integrated column amount from the sounding. Discrepancies between the sonde and satellite datasets decline two percentage points on average, compared to version 7 TOMS offsets. Second, the SHADOZ station data are compared to results of chamber simulations (JOSE-2000, Juelich Ozonesonde Intercomparison Experiment) in which the various SHADOZ techniques were evaluated. The range of JOSE column deviations from a standard instrument (-10%) in the chamber resembles that of the SHADOZ station data. It appears that some systematic variations in the SHADOZ ozone record are accounted for by differences in solution strength, data processing and instrument type (manufacturer).

As part of the TRACE-P mission, ozone vertical profile measurements were made at a number of locations in the North Pacific. At most of the sites there is also a multi-year record of ozonesonde observations. From seven locations in the western Pacific (Hong Kong; Taipei; Jeju Island, Korea; and Naha, Kagoshima, Tsukuba, and Sapporo, Japan), a site in the central Pacific (Hilo, HI), and a site on the west coast of the U.S. (Trinidad Head, CA) both a seasonal and event specific picture of tropospheric ozone over the North Pacific emerges. At all of the sites there is a pronounced spring maximum through the troposphere. There are, however, differences in the timing and strength of this feature. Over Japan the northward movement of the jet during the spring and summer influences the timing of the seasonal maximum. The ozone profiles suggest that transport of ozone rich air from the stratosphere plays a strong role in the development of this maximum. During March and April at Hong Kong ozone is enhanced in a layer that extends from the lower free troposphere into the upper troposphere that likely has its origin in biomass burning in northern Southeast Asia and equatorial Africa. During the winter the Pacific subtropical sites (latitude -25N) are dominated by air with a low-latitude, marine source that gives low ozone amounts particularly in the upper troposphere. In the summer in the boundary layer at all of the sites marine air dominates and ozone amounts are generally quite low (less than 25 ppb). The exception is near large population centers (Tokyo and Taipei but not Hong Kong) where pollution events can give amounts in excess of 80 ppb. During the TRACE-P intensive campaign period (February-April 2001) tropospheric ozone amounts were rather typical of those seen in the long-term records of the stations with multi-year soundings.

We present an analysis of the quasi-biennial oscillation (QBO) in tropical ozone using recent in situ measurements made by ozonesondes, supplemented by satellite profile and column data. The first in situ equatorial ozone profiles reveal the dramatic change in shape of the profile that accompanies the descent of the westerly shear zone. The partial pressure maximum in ozone increases by -25% in 5-6 months as it descends from 17.5 to 24 hPa. The amplitude of the QBO anomaly that extends from 15 to 80 hPa is found to exceed *20%, larger than indicated by earlier analyses of satellite data. The influence of the QBO on equatorial ozone is dominant between 10 and 45 hPa, but the seasonal cycle is more important below 50 hPa. The equatorial ozone anomalies are influenced by El Niiio-Southern Oscillation (ENSO) in the lowest part of the stratosphere. The ozone anomaly in the lower stratosphere at 20"s lags that at the equator by only a few months during the easterlies from 1994 to 1998, contrary to the previous picture of the subtropical and equatorial anomalies being out of phase.

A network of 12 southern hemisphere tropical and subtropical stations in the Southern Hemisphere ADditional OZonesondes (SHADOZ) project has provided over 2000 profiles of stratospheric and tropospheric ozone since 1998. Balloon-borne electrochemical concentration cell (ECC) ozonesondes are used with standard radiosondes for pressure, temperature and relative humidity measurements. The archived data are available at:http: //croc.gsfc.nasa.gov/shadoz. In Thompson et al., accuracies and imprecisions in the SHADOZ 1998- 2000 dataset were examined using ground-based instruments and the TOMS total ozone measurement (version 7) as references. Small variations in ozonesonde technique introduced possible biases from station-to-station. SHADOZ total ozone column amounts are now compared to version 8 TOMS; discrepancies between the two datasets are reduced 2\% on average. An evaluation of ozone variations among the stations is made using the results of a series of chamber simulations of ozone launches (JOSIE-2000, Juelich Ozonesonde Intercomparison Experiment) in which a standard reference ozone instrument was employed with the various sonde techniques used in SHADOZ. A number of variations in SHADOZ ozone data are explained when differences in solution strength, data processing and instrument type (manufacturer) are taken into account.

The first view of lower stratospheric and upper tropospheric structure from sondes is provided by a 3-year, 10-site record from the Southern Hemisphere ADditional OZonesondes (SHADOZ) network: http://code9 16.gsfc.nasa.gov/Data_services/shadoz. Observations covering 1998-2000 were made over Ascension Island; Nairobi, Kenya; Irene, South Africa; La Reunion Island; Watukosek, Java; Fiji; Tahiti; American Samoa; San Cristobal, Galapagos; Natal, Brazil. Taking the UT/LS (upper troposphere-lower stratosphere) as the region between 12 and 17 km, we examine ozone variability in this region on a week-to- week and seasonal basis. The tropopause is lower in September-October-November than in March-April-May, when ozone is a minimum at most SHADOZ stations. A zonal wave-one pattern (referring to ozone mixing ratios greater over the Atlantic and adjacent continents than over the Pacific and eastern Indian Ocean), persists all year. The wave, predominantly in the troposphere and with variable magnitude, appears to be due to general circulation - with subsidence over the Atlantic and frequent deep convection over the Pacific and Indian Ocean. The variability of deep convection - most prominent at Java, Fiji, Samoa and Natal - is explored in time-vs-altitude ozone curtains. Stratospheric incursions into the troposphere are most prominent in soundings at Irene and Reunion Island.

Over the past several years, we have developed two new tropospheric ozone retrievals from the TOMS (Total Ozone Mapping Spectrometer) satellite instrument that are of sufficient resolution to follow pollution episodes. The modified-residual technique uses v. 7 TOMS total ozone and is applicable to tropical regimes in which the wave-one pattern in total ozone is observed. The TOMS-direct method ('TDOT' = TOMS Direct Ozone in the Troposphere) represents a new algorithm that uses TOMS radiances directly to extract tropospheric ozone in regions of constant stratospheric ozone. It is not geographically restricted, using meteorological regimes as the basis for classifying TOMS radiances and for selecting appropriate comparison data. TDOT is useful where tropospheric ozone displays high mixing ratios and variability characteristic of pollution. Some of these episodes were observed downwind of Asian biomass burning during the TRACE-P (Transport and Atmospheric Chemical Evolution-Pacific) field experiment in March 2001. This paper features comparisons among TDOT tropospheric ozone column depth, integrated uv-DIAL measurements made from NASA's DC-8, and ozonesonde data.

The first view of lower stratospheric and upper tropospheric structure from sondes is provided by a 3-year, 10-site record from the Southern Hemisphere ADditional OZonesondes (SHADOZ) network: . Observations covering 1998-2000 were made over Ascension Island; Nairobi, Kenya; Irene, South Africa; Reunion Island; Watukosek, Java; Fiji; Tahiti; American Samoa; San Cristobal, Galapagos; Natal, Brazil. Taking the UT/LS (upper troposphere- lower stratosphere) as the region between 12 and 17 km, we examine ozone variability in this region on a week-to-week and seasonal basis. The tropopause is lower in September-October-November than in March-April-May, when ozone is a minimum at most SHADOZ stations. A zonal wave-one pattern (referring to ozone mixing ratios greater over the Atlantic and adjacent continents than over the Pacific and eastern Indian Ocean), persists all year. The wave, predominantly in the troposphere and with variable magnitude, appears to be due to general circulation - with subsidence over the Atlantic and frequent deep convection over the Pacific and Indian Ocean. The variability of deep convection most prominent at Java, Fiji, Samoa and Natal - is explored in time-vs-altitude ozone curtains. Stratospheric incursions into the troposphere are most prominent in soundings at Irene and Reunion Island.

The first view of stratospheric and tropospheric ozone variability in the southern hemisphere tropics is provided by a 3-year, 10-site record of ozone soundings from the Southern Hemisphere ADditional OZonesondes (SHADOZ) network. Observations covering 1998-2000 were made over Ascension Island; Nairobi, Kenya; Irene, South Africa; Reunion Island; Watukosek, Java; Fiji; Tahiti; American Samoa; San Cristobal, Galapagos; Natal, Brazil. Taking the TTL (tropical tropopause layer) as the region between 12 and 17 km, we examine ozone variability in this region on a week-to-week and seasonal basis. The TTL layer is lower in September-October-November than in March-April-May, when ozone is a minimum at most SHADOZ stations. A zonal wave-one pattern is apparent in column-integrated TTL ozone because ozone mixing ratios are greater over the Atlantic and adjacent continents than over the Pacific and eastern Indian Ocean. The wave-one persists all year with varying magnitude and appears to be due to general circulation - with subsidence over the Atlantic and frequent deep convection over the Pacific and Indian Ocean. The variability of deep convection - most prominent at Java, Fiji, Samoa and Natal - is explored in time-vs-altitude ozone curtains. Stratospheric incursions into the troposphere are most prominent in soundings at Irene and Reunion Island.

Ten data sets covering the period 1954-2000 are analyzed to show a 1% per year increase in stratospheric water vapor. The trend has persisted for at least 45 years, hence is unlikely the result of a single event but rather indicative of long-term climate change. A long-term change in the transport of water vapor into the stratosphere is the most probable cause.

As part of the SAFARI-2000 campaign, additional launches of ozonesondes were made at Irene, South Africa and at Lusaka, Zambia. These represent campaign augmentations to the SHADOZ database described in this paper. This network of 10 southern hemisphere tropical and subtropical stations, designated the Southern Hemisphere ADditional OZonesondes (SHADOZ) project and established from operational sites, provided over 1000 profiles from ozonesondes and radiosondes during the period 1998-2000. (Since that time, two more stations, one in southern Africa, have joined SHADOZ). Archived data are available at: http://code9l6.gsfc.nasa.gov/Data-services/shadoz>. Uncertainties and accuracies within the SHADOZ ozone data set are evaluated by analyzing: (1) imprecisions in stratospheric ozone profiles and in methods of extrapolating ozone above balloon burst; (2) comparisons of column-integrated total ozone from sondes with total ozone from the Earth-Probe/TOMS (Total Ozone Mapping Spectrometer) satellite and ground-based instruments; (3) possible biases from station-to-station due to variations in ozonesonde characteristics. The key results are: (1) Ozonesonde precision is 5%; (2) Integrated total ozone column amounts from the sondes are in good agreement (2-10%) with independent measurements from ground-based instruments at five SHADOZ sites and with overpass measurements from the TOMS satellite (version 7 data). (3) Systematic variations in TOMS-sonde offsets and in groundbased-sonde offsets from station to station reflect biases in sonde technique as well as in satellite retrieval. Discrepancies are present in both stratospheric and tropospheric ozone. (4) There is evidence for a zonal wave-one pattern in total and tropospheric ozone, but not in stratospheric ozone.

Ozone vertical profile measurements obtained from ozonesondes flown at Fiji, Samoa, Tahiti and the Galapagos are used to characterize ozone in the troposphere over the tropical Pacific. There is a significant seasonal variation at each of these sites. At sites in both the eastern and western Pacific, ozone is highest at almost all levels in the troposphere during the September-November season and lowest during, March-May. There is a relative maximum at all of the sites in the mid-troposphere during all seasons of the year (the largest amounts are usually found near the tropopause). This maximum is particularly pronounced during, the September-November season. On average, throughout the troposphere at all seasons, the Galapagos has larger ozone amounts than the western Pacific sites. A trajectory climatology is used to identify the major flow regimes that are associated with the characteristic ozone behavior at various altitudes and seasons. The enhanced ozone seen in the mid-troposphere during September-November is associated with flow from the continents. In the western Pacific this flow is usually from southern Africa (although 10-day trajectories do not always reach the continent), but also may come from Australia and Indonesia. In the Galapagos the ozone peak in the mid-troposphere is seen in flow from the South American continent and particularly from northern Brazil. The time of year and flow characteristics associated with the ozone mixing ratio peaks seen in both the western and eastern Pacific suggest that these enhanced ozone values result from biomass burning. In the upper troposphere low ozone amounts are seen with flow that originates in the convective western Pacific.

Vertical ozone profiles between the Equator and 10 S latitude available from the Southern Hemisphere Additional Ozone (SHADOZ) program provide consistent data Ozone sets from up to 10 sounding locations. SHADOZ designed to provide independent ozone profiles in the tropics for evaluation of satellite ozone data and models has made available over 600 soundings over the period 1998-1999. These observations provide an ideal data base for the detailed description of ozone and afford differential comparison between sites. TOMS total ozone when compared with correlative integrated total ozone overburden from the sondes is found to be negatively biased when using the classical constant mixing ratio procedure to determine residual ozone. On the other hand, the climatological method proposed by McPeters and Labow appears to give consistent results but is positively biased. The longer then two years series of measurements also was subjected to harmonic analysis to examine data cycles. These will be discussed as well.

During the Aerosols-99 trans-Atlantic cruise from Norfolk, VA, to Cape Town, South Africa, 22 ozonesondes were launched from the NOAA R/V R H Brown between 17 Jan and 6 Feb 1999, with all sondes but one reaching 30 km. A composite of ozone profiles along the transect shows high free tropospheric ozone (up to 100 ppbv at 9 km) between 5N and 20S, a coherent feature straddling either side of the ITCZ. Latitudinal variations of tropospheric ozone are interpreted using correlative measurements of surface ozone, CO, water vapor, and aerosol optical thickness (column absorbance) measured from the ship. Elevated ozone in the lower troposphere results from photochemical reactions of precursors emitted by biomass burning north of the ITCZ. However, the greatest ozone mixing ratios are in the mid-troposphere south of the ITCZ, which gives evidence of interhemispheric transport. Column-integrated tropospheric ozone, 35 DU from 0-16 km, agrees with that derived from the TOMS satellite by the modified-residual method [Thompson and Hudson, 1999]. NCEP wind fields, ship-launched radiosondes and back trajectories are consistent with a picture of recirculating air parcels centered in the tropical Atlantic region which is identified with the maximum wave-one amplitude in total ozone seen in sondes and by satellite.

We present the results of two independent analyses of ozonesonde measurements of the vertical profile of ozone. For most of the ozonesonde stations we use data that were recently reprocessed and reevaluated to improve their quality and internal consistency. The two analyses give similar results for trends in ozone. We attribute differences in results primarily to differences in data selection criteria and in utilization of data correction factors, rather than in statistical trend models. We find significant decreases in stratospheric ozone at all stations in middle and high latitudes of the northern hemisphere from 1970 to 1996, with the largest decreases located between 12 and 21 km, and trends of -3 to -10 %/decade near 17 km. The decreases are largest at the Canadian and the most northerly Japanese station, and are smallest at the European stations, and at Wallops Island, U.S.A. The mean mid-latitude trend is largest, -7 %/decade, from 12 to 17.5 km for 1970-96. For 1980-96, the decrease is more negative by 1-2 %/decade, with a maximum trend of -9 %/decade in the lowermost stratosphere. The trends vary seasonally from about 12 to 17.5 km, with largest ozone decreases in winter and spring. Trends in tropospheric ozone are highly variable and depend on region. There are decreases or zero trends at the Canadian stations for 1970-96, and decreases of -2 to -8 %/decade for the mid-troposphere for 1980-96; the three European stations show increases for 1970-96, but trends are close to zero for two stations for 1980-96 and positive for one; there are increases in ozone for the three Japanese stations for 1970-96, but trends are either positive or zero for 1980-96; the U.S. stations show zero or slightly negative trends in tropospheric ozone after 1980. It is not possible to define reliably a mean tropospheric ozone trend for northern mid-latitudes, given the small number of stations and the large variability in trends. The integrated column trends derived from the sonde data are consistent with trends derived from both surface based and satellite measurements of the ozone column.

This paper describes the validation of ozone data from the Upper Atmosphere Research Satellite (UARS) Microwave Limb Sounder (MLS). The MLS ozone retrievals are obtained from the calibrated microwave radiances (emission spectra) in two separate bands, at frequencies near 205 and 183 GHz. Analyses described here focus on the MLS Version 3 data (the first set of files made publicly available). We describe results of simulations performed to assess the quality of the retrieval algorithms, in terms of both mixing ratio and radiance closure. From actual MLS observations, the 205-GHz ozone retrievals give better closure (smaller radiance residuals) than that from the 183-GHz measurements and should be considered more accurate from the calibration aspects. However, the 183-GHz data are less noise limited in the mesosphere and can provide the most useful scientific results in that region. We compare the retrieved 205-GHz ozone profiles in the middle-to lower stratosphere to ozonesonde measurements at a wide range of latitudes and seasons. Ground-based lidar data from Table Mountain, California, provide a good reference for comparisons at higher altitudes. Based on these analyses, comparisons with balloon-borne measurements and others, as well as a detailed budget of estimated uncertainties, MLS results appear to be generally of high quality, with some biases worth mentioning. Results for the lowermost stratosphere (approx. 50 to 100 bPa) are still in need of improvement. A set of estimated precision and accuracy values is derived for the MLS ozone data sets. We also comment on recent updates in the retrieval algorithms and their impact on ozone values.

The Upper Atmosphere Research Satellite (UARS) microwave limb sounder (MLS) makes measurements of thermal emission at 183.3 GHz which are used to infer the concentration of water vapor over a pressure range of 46-0.2hPa (approximately 20-60 km). We provide a validation of MLS H2O by analyzing the integrity of the measurements, by providing an error characterization, and by comparison with data from other instruments. It is estimated that version 3 MLS H2O retrievals are accurate to within 20-25% in the lower stratosphere and to within 8-13% in the upper stratosphere and lower mesosphere. The precision of a single profile is estimated to be approximately 0.15 parts per million by volume (ppmv) in the midstratosphere and 0.2 ppmv in the lower and upper stratosphere. In the lower mesosphere the estimate of a single profile precision is 0.25-0.45 ppmv. During polar winter conditions, H2O retrievals at 46 hPa can have a substantial contribution from climatology. The vertical resolution of MLS H2O retrievals is approximately 5 km.

We provide a validation of MLS H(sub 2)O by analyzing the integrity of the measurements, by providing an error characterization and by comparison with data from other instruments. This paper concerns the data validation of middle atmosphere distributions of H(sub 2)O as measured by the Midrowave Limb Sounder (MLS).

Important changes in the ozone vertical profile over South Pole, Antarctica have occurred both during the recent period of measurements, 1986-1991, and since an earlier set of soundings was carried out from 1967-1971. From the onset of the 'ozone hole' over Antarctica in the early 1980s, there has been a tendency for years with lower spring ozone amounts to alternate with years with somewhat higher (although still depleted) ozone amounts. Beginning in 1989 there have been three consecutive years of strong depletion although the timing of the breakdown of the vortex has varied from year to year. Comparison of the vertical profiles between the two periods of study reveals the dramatic decreases in the ozone amounts in the stratosphere between 15-21 km during the spring. In addition, it appears that summer values are also now much lower in this altitude region.

Electrochemical concentration cell (ECC) ozone-sonde observations, made in recent years at ten stations whose locations range from the Arctic to Antarctica, have yielded a self-consistent ozone data base from which mean seasonal and annual latitudinal ozone vertical distributions to 35 km have been derived. Ozone measurement uncertainties are estimated, and results are presented in the Bass-Paur (1985) ozone absorption coefficient scale adopted for use with Dobson ozone spectrophotometers January 1, 1992. The data should be useful for comparison with model calculations of the global distribution of atmospheric ozone, for serving as apriori statistical information in deriving ozone vertical distributions from satellite and Umkehr observations, and for improving the satellite and Umkehr ozone inversion algorithms. Attention is drawn to similar results based on a less comprehensive data set published in Ozone in the Atmosphere, Proceedings of the 1988 Quadrennial Ozone Symposium where errors in data tabulations occurred for three of the stations due to inadvertent transposition of ozone partial pressure and air temperature values.

This paper describes the validation of ozone data from the Upper Atmosphere Research Satellite (UARS) Microwave Limb Sounder (MLS). The MLS ozone retrievals are obtained from the calibrated microwave radiances (emission spectra) in two separate bands, at frequencies near 205 and 183 GHz.

Ozone profiles obtained at Boulder, Colorado and Wallops Island, Virginia indicate that ozone was about 25% below normal during the winter and spring of 1992-93 in the 12-22 km region. This large ozone reduction in the lower stratosphere, though sometimes partially compensated by higher than normal ozone above 24 km, was responsible for the low total column ozone values observed across the United States during this period. Normal temperatures throughout the low ozone region suggest that transport-related effects are probably not the most important cause of the ozone deficits. This region of low ozone at Boulder corresponds closely with the location of the enhanced H2SO4/H2O aerosol from the Pinatubo eruption of 1991 as measured near Boulder and at Laramie, Wyoming. Trajectory analyses suggest that except at low altitudes in spring, air parcels on the days of the ozone measurements generally arrived at Boulder from higher latitude, although seldom higher than 60 deg N, and hence may have been subjected to heterogeneous chemical processing on the surface of Pinatubo aerosol droplets resulting in chlorine-catalyzed ozone destruction, a process which is believed to be more effective under the lower winter temperatures and sunlight levels of higher latitudes.

It is shown here that surface ozone concentrations at the South Pole in the austral summer decreased by 17 percent over the period 1976-90. Over the same period, solar irradiance at the South Pole in January and February decreased by 7 percent as a result of a 25 percent increase in cloudiness. It is suggested that the trend in the summer ozone concentrations is caused by enhanced photochemical destruction of ozone in the lower troposphere caused by the increased penetration of UV radiation associated with stratospheric ozone depletion, coupled with enhanced transport of ozone-poor marine air from lower latitudes to the South Pole.