Ozone Record Research Articles

Reconciliation of halogen-induced ozone loss with the total-column ozone record

The observed depletion of the stratospheric ozone layer from the 1980s onwards is attributed to halogens released through human activities. Model simulations show that stratospheric ozone loss has declined by over 10% since stratospheric halogen loading peaked in the late 1990s, indicating that the recovery of the ozone layer is well under way.

Evaluation of the use of five laboratory-determined ozone absorption cross sections in Brewer and Dobson retrieval algorithms

Abstract. The primary ground-based instruments used to report total column ozone (TOC) are Brewer and Dobson spectrophotometers in separate networks. These instruments make measurements of the UV irradiances, and through a well-defined process, a TOC value is produced. Inherent to the algorithm is the use of a laboratory-determined cross-section data set. We used five ozone cross-section data sets: three data sets that are based on measurements of Bass and Paur; one derived from Daumont, Brion and Malicet (DBM); and a new set determined by Institute of Experimental Physics (IUP), University of Bremen. The three Bass and Paur (1985) sets are as follows: quadratic temperature coefficients from the IGACO (a glossary is provided in Appendix A) web page (IGQ4), the Brewer network operational calibration set (BOp), and the set used by Bernhard et al. (2005) in the reanalysis of the Dobson absorption coefficient values (B05). The ozone absorption coefficients for Brewer and Dobson instruments are then calculated using the normal Brewer operative method, which is essentially the same as that used for Dobson instruments. Considering the standard TOC algorithm for the Brewer instruments and comparing to the Brewer standard operational calibration data set, using the slit functions for the individual instruments, we find the IUP data set changes the calculated TOC by −0.5%, the DBM data set changes the calculated TOC by −3.2%, and the IGQ4 data set at −45 °C changes the calculated TOC by +1.3%. Considering the standard algorithm for the Dobson instruments, and comparing to results using the official 1992 ozone absorption coefficients values and the single set of slit functions defined for all Dobson instruments, the calculated TOC changes by +1%, with little variation depending on which data set is used. We applied the changes to the European Dobson and Brewer reference instruments during the Izaña 2012 Absolute Calibration Campaign. With the application of a common Langley calibration and the IUP cross section, the differences between Brewer and Dobson data sets vanish, whereas using those of Bass and Paur and DBM produces differences of 1.5 and 2%, respectively. A study of the temperature dependence of these cross-section data sets is presented using the Arosa, Switzerland, total ozone record of 2003–2006, obtained from two Brewer-type instruments and one Dobson-type instrument, combined with the stratospheric ozone and temperature profiles from the Payerne soundings in the same period. The seasonal dependence of the differences between the results from the various instruments is greatly reduced with the application of temperature-dependent absorption coefficients, with the greatest reduction obtained using the IUP data set.

Solar Backscatter UV (SBUV) total ozone and profile algorithm

Abstract. We describe the algorithm that has been applied to develop a 42 yr record of total ozone and ozone profiles from eight Solar Backscatter UV (SBUV) instruments launched on NASA and NOAA satellites since April 1970. The Version 8 (V8) algorithm was released more than a decade ago and has been in use since then at NOAA to produce their operational ozone products. The current algorithm (V8.6) is basically the same as V8, except for updates to instrument calibration, incorporation of new ozone absorption cross-sections, and new ozone and cloud height climatologies. Since the V8 algorithm has been optimized for deriving monthly zonal mean (MZM) anomalies for ozone assessment and model comparisons, our emphasis in this paper is primarily on characterizing the sources of errors that are relevant for such studies. When data are analyzed this way the effect of some errors, such as vertical smoothing of short-term variability, and noise due to clouds and aerosols diminish in importance, while the importance of others, such as errors due to vertical smoothing of the quasi-biennial oscillation (QBO) and other periodic and aperiodic variations, become more important. With V8.6 zonal mean data we now provide smoothing kernels that can be used to compare anomalies in SBUV profile and partial ozone columns with models. In this paper we show how to use these kernels to compare SBUV data with Microwave Limb Sounder (MLS) ozone profiles. These kernels are particularly useful for comparisons in the lower stratosphere where SBUV profiles have poor vertical resolution but partial column ozone values have high accuracy. We also provide our best estimate of the smoothing errors associated with SBUV MZM profiles. Since smoothing errors are the largest source of uncertainty in these profiles, they can be treated as error bars in deriving interannual variability and trends using SBUV data and for comparing with other measurements. In the V8 and V8.6 algorithms we derive total column ozone by integrating the SBUV profiles, rather than from a separate set of wavelengths, as was done in previous algorithm versions. This allows us to extend the total ozone retrieval to 88° solar zenith angle (SZA). Since the quality of total column data is affected by reduced sensitivity to ozone in the lower atmosphere by cloud and Rayleigh attenuation, which gets worse with increasing SZA, we provide our best estimate of these errors, as well as the kernels that can be used to test the sensitivity of the derived columns to long-term changes in ozone in the lower atmosphere.

A comparison of 40 years of SBUV measurements of column ozone with data from the Dobson/Brewer network

AbstractTotal column ozone data from the Nimbus‐4 Backscatter UltraViolet (BUV) instrument, Nimbus‐7 Solar Backscatter Ultraviolet (SBUV) instrument, as well as from seven NOAA SBUV/2 instruments have been newly reprocessed with the Version 8.6 ozone retrieval algorithm. This yields a coherent data set that, unlike the Total Ozone Mapping Spectrometer ozone record, has no data gaps or significant time periods with large uncertainties due to calibration issues from 1979 to the present. The column ozone data from the first 3 years of the BUV record (1970–1972) is of high quality and can be used to extend the satellite ozone record back over 40 years. With the new algorithm, an improved total column ozone value is calculated by summing up the profile information as opposed to a single direct column measurement, and the algorithm is optimized for the detection of long‐term trends. The results from this processing of these data have been systematically compared to total ozone data from Brewer and Dobson spectrophotometers for many individual ground stations as a function of time, satellite solar zenith angle, and latitude. The time series comparisons show an agreement within ± 1% over the past 40 years with the bias approaching zero over the last decade. The aerosols associated with the eruption of Mt Pinatubo in 1991 produced an underestimation of ozone for our retrievals at high slant columns while the near‐nadir values were relatively unaffected. There is very little systematic offset between the satellite and ground‐based measurements as a function of latitude with the Nimbus‐4 BUV data (1970–1976) showing the largest offsets. The comparisons as a function of satellite solar zenith angle show consistent behavior for all instruments. Comparisons with ozonesonde data show good agreement in the integrated column up to 25 hPa with differences of no more than 5%.

Comparative Spectral Analysis and Correlation Properties of Observed and Simulated Total Column Ozone Records

We present a statistical analysis of total column ozone records obtained from satellite measurements and from two global climate chemistry models on global scale. Firstly, a spectral weight analysis is performed where the relative strength of semiannual, annual and quasi-biennial oscillations are determined with respect to the integrated power spectra. The comparison reveals some anomalies in the model representations at each spectral component. The tails of the spectra demonstrate that both models underestimate high frequency (daily) ozone variability, which might have a complex origin, since several dynamical processes affect short time changes of the ozone level at a given location. Secondly, detrended fluctuation analysis is exploited to analyze two-point correlations of anomaly time series. Both models reproduce the characteristic geographic dependence of correlation strength over the overlapping area with empirical observations (latitude band between 60°S and 60°N). The values of precise correlation exponents are hard to obtain over regions where quasi-biennial oscillations or other strong nonstationarities (ozone hole) are present. In spite of all the numerical difficulties, significant long range correlations are detected for total ozone over all geographic locations.

Characterization of Odin-OSIRIS ozone profiles with the SAGE II dataset

Abstract. The Optical Spectrograph and InfraRed Imaging System (OSIRIS) on board the Odin spacecraft has been taking limb-scattered measurements of ozone number density profiles from 2001–present. The Stratospheric Aerosol and Gas Experiment II (SAGE II) took solar occultation measurements of ozone number densities from 1984–2005 and has been used in many studies of long-term ozone trends. We present the characterization of OSIRIS SaskMART v5.0× against the new SAGE II v7.00 ozone profiles for 2001–2005, the period over which these two missions had overlap. This information can be used to merge OSIRIS with SAGE II into a single ozone record from 1984 to the present, if other satellite ozone measurements are included to account for gaps in the OSIRIS dataset in the winter hemisphere. Coincident measurement pairs were selected for ±1 h, ±1° latitude, and ±500 km. The absolute value of the resulting mean relative difference profile is <5% for 13.5–54.5 km and <3% for 24.5–53.5 km. Correlation coefficients R > 0.9 were calculated for 13.5–49.5 km, demonstrating excellent overall agreement between the two datasets. Coincidence criteria were relaxed to maximize the number of measurement pairs and the conditions under which measurements were taken. With the broad coincidence criteria, good agreement (< 5%) was observed under most conditions for 20.5–40.5 km. However, mean relative differences do exceed 5% for several cases. Above 50 km, differences between OSIRIS and SAGE II are partly attributed to the diurnal variation of ozone. OSIRIS data are biased high compared with SAGE II at 22.5 km, particularly at high latitudes. Dynamical coincidence criteria, using derived meteorological products, were also tested and yielded similar overall results, with slight improvements to the correlation at high latitudes. The OSIRIS optics temperature is low (<16 °C) during May–July, when the satellite enters the Earth's shadow for part of its orbit. During this period, OSIRIS measurements are biased low by 5–12% for 27.5–38.5 km. Biases between OSIRIS ascending node (northward equatorial crossing time ~18:00 LT – local time) and descending node (southward equatorial crossing time ~06:00 LT) measurements are also noted under some conditions. This work demonstrates that OSIRIS and SAGE II have excellent overall agreement and characterizes the biases between these datasets.

Geophysical validation and long-term consistency between GOME-2/MetOp-A total ozone column and measurements from the sensors GOME/ERS-2, SCIAMACHY/ENVISAT and OMI/Aura

Abstract. The main aim of the paper is to assess the consistency of five years of Global Ozone Monitoring Experiment-2/Metop-A [GOME-2] total ozone columns and the long-term total ozone satellite monitoring database already in existence through an extensive inter-comparison and validation exercise using as reference Brewer and Dobson ground-based measurements. The behaviour of the GOME-2 measurements is being weighed against that of GOME (1995–2011), Ozone Monitoring Experiment [OMI] (since 2004) and the Scanning Imaging Absorption spectroMeter for Atmospheric CartograpHY [SCIAMACHY] (since 2002) total ozone column products. Over the background truth of the ground-based measurements, the total ozone columns are inter-evaluated using a suite of established validation techniques; the GOME-2 time series follow the same patterns as those observed by the other satellite sensors. In particular, on average, GOME-2 data underestimate GOME data by about 0.80%, and underestimate SCIAMACHY data by 0.37% with no seasonal dependence of the differences between GOME-2, GOME and SCIAMACHY. The latter is expected since the three datasets are based on similar DOAS algorithms. This underestimation of GOME-2 is within the uncertainty of the reference data used in the comparisons. Compared to the OMI sensor, on average GOME-2 data underestimate OMI_DOAS (collection 3) data by 1.28%, without any significant seasonal dependence of the differences between them. The lack of seasonality might be expected since both the GOME data processor [GDP] 4.4 and OMI_DOAS are DOAS-type algorithms and both consider the variability of the stratospheric temperatures in their retrievals. Compared to the OMI_TOMS (collection 3) data, no bias was found. We hence conclude that the GOME-2 total ozone columns are well suitable to continue the long-term global total ozone record with the accuracy needed for climate monitoring studies.

Development of a climate record of tropospheric and stratospheric column ozone from satellite remote sensing: evidence of an early recovery of global stratospheric ozone

Abstract. Ozone data beginning October 2004 from the Aura Ozone Monitoring Instrument (OMI) and Aura Microwave Limb Sounder (MLS) are used to evaluate the accuracy of the Cloud Slicing technique in effort to develop long data records of tropospheric and stratospheric ozone and for studying their long-term changes. Using this technique, we have produced a 32-yr (1979–2010) long record of tropospheric and stratospheric column ozone from the combined Total Ozone Mapping Spectrometer (TOMS) and OMI. Analyses of these time series suggest that the quasi-biennial oscillation (QBO) is the dominant source of inter-annual variability of stratospheric ozone and is clearest in the Southern Hemisphere during the Aura time record with related inter-annual changes of 30–40 Dobson Units. Tropospheric ozone for the long record also indicates a QBO signal in the tropics with peak-to-peak changes varying from 2 to 7 DU. The most important result from our study is that global stratospheric ozone indicates signature of a recovery occurring with ozone abundance now approaching the levels of year 1980 and earlier. The negative trends in stratospheric ozone in both hemispheres during the first 15 yr of the record are now positive over the last 15 yr and with nearly equal magnitudes. This turnaround in stratospheric ozone loss is occurring about 20 yr earlier than predicted by many chemistry climate models. This suggests that the Montreal Protocol which was first signed in 1987 as an international agreement to reduce ozone destroying substances is working well and perhaps better than anticipated.

Spatial-temporal variations in surface ozone in Northern China as observed during 2009–2010 and possible implications for future air quality control strategies

Abstract. The Project of Atmospheric Combined Pollution Monitoring over Beijing and its Surrounding Areas, was an intensive field campaign conducted over Northern China between June 2009 and August 2011 to provide a comprehensive record of ozone (O3) and nitrogen oxides (NOx) and contribute to an in-depth understanding of air pollution in Northern China and its driving forces. In this campaign, 25 stations in an air-quality monitoring network provided regional-scale spatial coverage. In this study, we analyzed the data on O3 and NOx levels obtained at 22 sites (out of 25 sites due to data availability) over Northern China between 1 September 2009 and 31 August 2010. Our goal was to investigate the O3 spatial-temporal variations and control strategy in this area. Significant diurnal and seasonal variations were noted, with the highest concentrations typically found at around 03:00 p.m. (local time) and in June. The lowest concentrations were generally found during early morning hours (around 06:00 a.m.) and in December. Compared with July and August, June has increased photochemical production due to decreased cloud cover coupled with reduced O3 loss due to less dry deposition, inducing an O3 peak appearing in June. The averaged O3 concentrations were lower in the plains area compared with the mountainous area due to the titration effects of high NOx emissions in urban areas. When the characteristics of O3 pollution in different regions were distinguished by factor analysis, we found high levels of O3 that exceeded China's National Standard throughout the plains, especially over Beijing and the surrounding areas. An integrated analysis with emissions data, meteorological data, and topography over Northern China found that the meteorological conditions were the main factors that dominated the spatial variations of O3, with the presence of abundant emissions of precursors in this area. The smog production algorithm and space-based HCHO/NO2 column ratio were used to show the O3-NOx-VOCs sensitivity and examine the control strategy of O3 over Northern China. The results show that summer O3 production in the plains and northern mountainous areas was sensitive to VOCs and NOx, respectively. The presented results are intended to provide guidance for redefining government strategies to control the photochemical formation of air pollutants over Northern China and are relevant for developing urban agglomerations worldwide.

Total ozone and surface UV trends in the United Kingdom: 1979–2008

AbstractIn this study we present the UK's total ozone and UV data records, their measurement and preliminary processing, and discuss the observed trends. Notably, we combine the records from the Camborne and Reading sites to obtain a single ozone data series for southern England—a total duration of 30 years.Two‐section linear trends and cross‐over years are determined for Lerwick and southern England, both annually and seasonally. The observed minimum using this technique in the UK ozone record is found to occur during the year 1993. Significant trends of − 4.8% per decade for southern England and − 5.8% per decade for Lerwick are seen prior to the mid‐1990s; the rate of decrease in the UK being at the upper limit of other European stations. No significant ozone trend is seen for the latter period in either location in contrast with Europe as a whole. We, additionally, compare the satellite‐derived total ozone trends for both locations.The UV record at Reading showed a significant trend from 1993 to 2008 in the daily maximum UV index record (6.6% per decade), despite no significant recovery in the total ozone data series, suggesting a reduction in cloud cover during the midday period. Filtering data to remove other factors shows the erythemal UV to have an ozone‐dependent trend of − 0.11% per year, but this is not statistically significant. We find no correlation between anomalies in the surface UV and total ozone records suggesting that the majority of the inter‐annual variability is due to changes in cloud cover and other effects. Copyright © 2011 Royal Meteorological Society

Extreme events in total ozone over the Northern mid-latitudes: an analysis based on long-term data sets from five European ground-based stations

We apply methods from extreme value theory to identify extreme events in high (termed EHOs) and low (termed ELOs) total ozone and to describe the distribution tails (i.e. very high and very low values) of five long-term European ground-based total ozone time series. The influence of these extreme events on observed mean values, long-term trends and changes is analysed. The results show a decrease in EHOs and an increase in ELOs during the last decades, and establish that the observed downward trend in column ozone during the 1970–1990s is strongly dominated by changes in the frequency of extreme events. Furthermore, it is shown that clear ‘fingerprints’ of atmospheric dynamics (NAO, ENSO) and chemistry [ozone depleting substances (ODSs), polar vortex ozone loss] can be found in the frequency distribution of ozone extremes, even if no attribution is possible from standard metrics (e.g. annual mean values). The analysis complements earlier analysis for the world’s longest total ozone record at Arosa, Switzerland, confirming and revealing the strong influence of atmospheric dynamics on observed ozone changes. The results provide clear evidence that in addition to ODS, volcanic eruptions and strong/moderate ENSO and NAO events had significant influence on column ozone in the European sector.

Extreme events in total ozone over Arosa – Part 2: Fingerprints of atmospheric dynamics and chemistry and effects on mean values and long-term changes

Abstract. In this study the frequency of days with extreme low (termed ELOs) and extreme high (termed EHOs) total ozone values and their influence on mean values and trends are analyzed for the world's longest total ozone record (Arosa, Switzerland). The results show (i) an increase in ELOs and (ii) a decrease in EHOs during the last decades and (iii) that the overall trend during the 1970s and 1980s in total ozone is strongly dominated by changes in these extreme events. After removing the extremes, the time series shows a strongly reduced trend (reduction by a factor of 2.5 for trend in annual mean). Excursions in the frequency of extreme events reveal "fingerprints" of dynamical factors such as ENSO or NAO, and chemical factors, such as cold Arctic vortex ozone losses, as well as major volcanic eruptions of the 20th century (Gunung Agung, El Chichón, Mt. Pinatubo). Furthermore, atmospheric loading of ozone depleting substances leads to a continuous modification of column ozone in the Northern Hemisphere also with respect to extreme values (partly again in connection with polar vortex contributions). Application of extreme value theory allows the identification of many more such "fingerprints" than conventional time series analysis of annual and seasonal mean values. The analysis shows in particular the strong influence of dynamics, revealing that even moderate ENSO and NAO events have a discernible effect on total ozone. Overall the approach to extremal modelling provides new information on time series properties, variability, trends and the influence of dynamics and chemistry, complementing earlier analyses focusing only on monthly (or annual) mean values.

Year‐round record of surface ozone at coastal (Dumont d'Urville) and inland (Concordia) sites in East Antarctica

Surface ozone is measured since 2004 at the coastal East Antarctic station of Dumont d'Urville (DDU) and since 2007 at the Concordia station located on the high East Antarctic plateau. Ozone levels at Concordia reach a maximum of 35 ppbv in July and a minimum of 21 ppbv in February. From November to January, sudden increases of the ozone level, up to 15–20 ppbv above average, often take place. They are attributed to local photochemical ozone production as previously seen at the South Pole. The detailed examination of the diurnal ozone record in summer at Concordia suggests a local photochemical ozone production of around 0.2 ppbv h−1 during the morning. The ozone record at DDU exhibits a maximum of 35 ppbv in July and a minimum of 18 ppbv in January. Mixing ratios at DDU are always higher than those at Neumayer (NM), another coastal Antarctic station. A noticeable difference in the ozone records at the two coastal sites lies in the larger ozone depletion events occurring from July to September at NM compared to DDU, likely due to stronger BrO episodes in relation with a larger sea ice coverage offshore that site. A second difference is the large day‐to‐day fluctuations which are observed from November to January at DDU but not at NM. That is attributed to a stronger impact at DDU than at NM of air masses coming from the Antarctic plateau. The consequences of such a high oxidizing property of the atmosphere over East Antarctica are discussed with regard to the dimethylsulfide (DMS) chemistry.

Technical Note: A SAGE-corrected SBUV zonal-mean ozone data set

Abstract. A stratospheric vertically resolved, monthly, zonal-mean ozone data set based on Satellite Aerosol and Gas Experiment (SAGE) and Solar Backscatter UltraViolet (SBUV) data spanning 1979–2005 is presented. Drifts in individual SBUV instruments and inter-SBUV biases are corrected using SAGE I and II by calculating differences between coincident SAGE-SBUV measurements. In this way the daily, near-global coverage of SBUV(/2) is combined with the stability and precision of SAGE to provide a homogeneous ozone record suitable for trend analysis. The resultant SAGE-corrected SBUV data set, shows, for example, a more realistic Quasi-Biennial Oscillation signal compared to the one derived from SBUV data alone. Furthermore, this methodology can be used to extend the present data set beyond the lifetime of SAGE II.

Increasing surface ozone concentrations in the background atmosphere of Southern China, 1994–2007

Abstract. Tropospheric ozone is of great importance with regard to air quality, atmospheric chemistry, and climate change. In this paper we report the first continuous record of surface ozone in the background atmosphere of South China. The data were obtained from 1994 to 2007 at a coastal site in Hong Kong, which is strongly influenced by the outflow of Asian continental air during the winter and the inflow of maritime air from the subtropics in the summer. Three methods are used to derive the rate of change in ozone. A linear fit to the 14-year record shows that the ozone concentration increased by 0.58 ppbv/yr, whereas comparing means in years 1994–2000 and 2001–2007 gives an increase of 0.87 ppbv/yr for a 7-year period. The ozone changes in air masses from various source regions are also examined. Using local wind and carbon monoxide (CO) data to filter out local influence, we find that ozone increased by 0.94 ppbv/yr from 1994–2000 to 2001–2007 in air masses from Eastern China, with similar changes in the other two continent-influenced air-mass groups, but no statistically significant change in the marine air. An examination of the nitrogen dioxide (NO2) column obtained from GOME and SCIAMACHY reveals an increase in atmospheric NO2 in China's three fastest developing coastal regions, whereas NO2 in other parts of Asia decreased during the same period, and no obvious trend over the main shipping routes in the South China Sea was indicated. Thus the observed increase in background ozone in Hong Kong is most likely due to the increased emissions of NO2 (and possibly volatile organic compounds (VOCs) as well) in the upwind coastal regions of mainland China. The CO data at Hok Tsui showed less definitive changes compared to the satellite NO2 column. The increase in background ozone likely made a strong contribution (81%) to the rate of increase in "total ozone" at an urban site in Hong Kong, suggesting the need to consider distant sources when developing long-term strategies to mitigate local ozone pollution.

Reassessment of causes of ozone column variability following the eruption of Mount Pinatubo using a nudged CCM

Abstract. The eruption of Mount Pinatubo produced the largest loading of stratospheric sulphate aerosol in the twentieth century. This heated the tropical lower stratosphere, affecting stratospheric circulation, and provided enhanced surface area for heterogeneous chemistry. These factors combined to produce record low values of "global" total ozone column. Though well studied, there remains some uncertainty about the attribution of this low ozone, with contributions from both chemical and dynamical effects. We take a complementary approach to previous studies, nudging the potential temperature and horizontal winds in the new UKCA chemistry climate model to reproduce the atmospheric response and assess the impact on global total ozone. We then combine model runs and observations to distinguish between chemical and dynamical effects. To estimate the effects of increased heterogeneous chemistry on ozone we compare runs with volcanically enhanced and background surface aerosol density. The modelled depletion of global ozone peaks at about 7 DU in early 1993, in good agreement with values obtained from observations. We subtract the modelled aerosol induced ozone loss from the observed ozone record and attribute the remaining variability to `dynamical' effects. The remaining variability is dominated by the QBO. We also examine tropical and mid-latitude ozone, diagnosing contributions from El Niño in the tropics and identifying dynamically driven low ozone in northern mid-latitudes, which we interpret as possible evidence of changes in the QBO. We conclude that, on a global scale, the record lows of extra-polar ozone are produced by the increased heterogeneous chemistry, although there is evidence for dynamics produced low ozone in certain regions, including northern mid-latitudes.

On the turnaround of stratospheric ozone trends deduced from the reevaluated Umkehr record of Arosa, Switzerland

In this work, we investigate the issue of the turnaround in ozone trends of the recently homogenized Umkehr ozone record of Arosa, Switzerland, which is the longest Umkehr data set, extending from 1956 to date, using different statistical methods. All methods show statistically significant negative ozone trends from 1970 to 1995 in the upper stratosphere (above 32.6 km) throughout the course of the year as well as in the lower stratosphere (below 23.5 km) mainly during winter to spring, which can be partially attributed to dynamical changes. Over the recent period (1996–2004) the year‐round trends in the lower stratosphere become positive and are more positive during the winter to spring period. The results also show changes in upper stratospheric ozone trends after 1996, which are, however, not statistically significant at 95% if aerosol correction is applied on the retrieved data. This lack of significant trend changes during the recent period in the upper stratosphere is regionally coherent with recent results derived from upper stratospheric ozone data recorded by lidars, microwave radiometers, and satellite instruments at an adjacent location. Although the positive change in trends after 1996 both for upper and lower stratospheric ozone is in line with the reduction of the emissions of ozone‐depleting substances from the successful implementation of the Montreal Protocol and its amendments, we recommend, because of lack of significance for the upper stratospheric trends, repeating this analysis in a few years in order to overcome ambiguous results for documentation of the turnaround of upper stratospheric ozone.

Re-evaluation of the 1950–1962 total ozone record from Longyearbyen, Svalbard

Abstract. The historical total ozone measurements taken with Dobson Spectrophotometer #8 at Longyearbyen (78.2° N, 15.6° E), Svalbard, Norway, in the period 1950–1962 have been re-analyzed and homogenized based on the original measurement logs, using present-day procedures. In lack of sufficient calibration information, an empirical quality assessment was performed, based on a climatological comparison with ozone measurements in Tromsø, using TOMS data at both sites in the period 1979–2001, and ground-based Dobson data in the period 1950–1962. The assessment revealed that the C wavelength pair direct-sun (DS) measurements are most trustworthy (and most frequent), while the WMO standard reference mode AD direct-sun has a systematic bias. Zenith-blue (ZB) measurements at solar zenith angles (SZA) <78° were adjusted to DS data using different empirical functions before and after 1957 (the start of the International Geophysical Year). ZB measurements at larger SZAs were homogenized by means of a normalization function derived from days with measurements over a wide range of SZAs. Zenith-cloudy measurements, which are particularly frequent during the summer months, were homogenized by applying correction factors depending on the cloud type (high thin clouds and medium to low thick clouds). The combination of all measurements yields a total of 4685 single values, covering 1637 days from September 1950 to September 1962; moon measurements during the polar night add another 137 daily means. The re-evaluated data show a convincing consistence with measurements since 1979 (TOMS, SAOZ, Dobson) as well as with the 1957–1962 data stored at the World Ozone and UV Data Centre (WOUDC).

Ten years of GOME/ERS‐2 total ozone data—The new GOME data processor (GDP) version 4: 1. Algorithm description

The Global Ozone Monitoring Instrument (GOME) was launched on European Space Agency's ERS‐2 platform in April 1995. The GOME data processor (GDP) operational retrieval algorithm has generated total ozone columns since July 1995. In 2004 the GDP system was given a major upgrade to version 4.0, a new validation was performed, and the 10‐year GOME level 1 data record was reprocessed. In two papers, we describe the GDP 4.0 retrieval algorithm and present an error budget and sensitivity analysis (paper 1) and validation of the GDP total ozone product and the overall accuracy of the entire GOME ozone record (paper 2). GDP 4.0 uses an optimized differential optical absorption spectroscopy (DOAS) algorithm, with air mass factor (AMF) conversions calculated using the radiative transfer code linearized discrete ordinate radiative transfer (LIDORT). AMF computation is based on the TOMS version 8 ozone profile climatology, classified by total column, and AMFs are adjusted iteratively to reflect the DOAS slant column result. GDP 4.0 has improved wavelength calibration and reference spectra and includes a new molecular Ring correction to deal with distortion of ozone absorption features due to inelastic rotational Raman scattering effects. Preprocessing for cloud parameter estimation in GDP 4.0 is done using two new cloud correction algorithms: OCRA and ROCINN. For clear and cloudy scenes the precision of the ozone column product is better than 2.4 and 3.3%, respectively, for solar zenith angles up to 80°. Comparisons with ground‐based data are generally at the 1–1.5% level or better for all regions outside the poles.

Measurements of Trace Gases in the Inflow of South China Sea Background Air and Outflow of Regional Pollution at Tai O, Southern China

We present a 16-month record of ozone (O3), carbon monoxide (CO), total reactive nitrogen (NO y ), sulphur dioxide (SO2), methane (CH4), C2 – C8 non-methane hydrocarbons (NMHCs), C1 – C2 halocarbons, and dimethyl sulfide (DMS) measured at a southern China coastal site. The study aimed to establish/update seasonal profiles of chemically active trace gases and pollution tracers in subtropical Asia and to characterize the composition of the `background' atmosphere over the South China Sea (SCS) and of pollution outflow from the industrialized Pearl River Delta (PRD) region and southern China. Most of the measured trace gases of anthropogenic origin exhibited a winter maximum and a summer minimum, while O3 showed a maximum in autumn which is in contrast to the seasonal behavior of O3 in rural eastern China and in many mid-latitude remote locations in the western Pacific. The data were segregated into two groups representing the SCS background air and the outflow of regional continental pollution (PRD plus southern China), based on CO mixing ratios and meteorological conditions. NMHCs and halocarbon data were further analyzed to examine the relationships between their variability and atmospheric lifetime and to elucidate the extent of atmospheric processing in the sampled air parcels. The trace gas variability (S) versus lifetime (τ) relationship, defined by the power law, S lnx = Aτ− b, (where X is the trace gas mixing ratio) gives a fit parameter A of 1.39 and exponent b of 0.42 for SCS air, and A of 2.86 and b of 0.31 for the regional continental air masses. An examination of ln[n-butane]/ln[ethane] versus ln[propane]/ln[ethane] indicates that their relative abundance was dominated by mixing as opposed to photochemistry in both SCS and regional outflow air masses. The very low ratios of ethyne/CO, propane/ethane and toluene/benzene suggest that the SCS air mass has undergone intense atmospheric processing since these gases were released into the atmosphere. Compared to the results from other polluted rural sites and from urban areas, the large values of these species in the outflow of PRD/southern China suggest source(s) emitting higher levels of ethyne, benzene, and toluene, relative to light alkanes. These chemical characteristics could be unique indicators of anthropogenic emissions from southern China.