Abstract. In June 2009, 22 spectrometers from 14 institutes measured tropospheric and stratospheric NO 2 from the ground for more than 11 days during the Cabauw Intercomparison Campaign of Nitrogen Dioxide measuring Instruments (CINDI), at Cabauw, NL (51.97 • N, 4.93 • E). All visible instruments used a common wavelength range and set of cross sections for the spectral analysis. Most of the instruments were of the multi-axis design with analysis by differential spectroscopy software (MAX-DOAS), whose nonzenith slant columns were compared by examining slopes of their least-squares straight line fits to mean values of a selection of instruments, after taking 30-min averages. Zenith slant columns near twilight were compared by fits Correspondence to: H. K. Roscoe (h.roscoe@bas.ac.uk) to interpolated values of a reference instrument, then normalised by the mean of the slopes of the best instruments. For visible MAX-DOAS instruments, the means of the fitted slopes for NO 2 and O 4 of all except one instrument were within 10% of unity at almost all non-zenith elevations, and most were within 5%. Values for UV MAX-DOAS instruments were almost as good, being 12% and 7%, respectively. For visible instruments at zenith near twilight, the means of the fitted slopes of all instruments were within 5% of unity. This level of agreement is as good as that of previous intercomparisons, despite the site not being ideal for zenith twilight measurements. It bodes well for the future of measurements of tropospheric NO 2 , as previous intercomparisons were only for zenith instruments focussing on stratospheric NO 2 , with their longer heritage.Published by Copernicus Publications on behalf of the European Geosciences Union.

Abstract. A long-term ozone loss time series is necessary to understand the evolution of ozone in Antarctica. Therefore, we construct the time series using ground-based, satellite and bias-corrected multi-sensor reanalysis (MSR) data sets for the period 1989–2010. The trends in ozone over 1979–2010 are also estimated to further elucidate its evolution in the wake of decreasing halogen levels in the stratosphere. Our analysis with ground-based observations shows that the average ozone loss in the Antarctic is about −33 to −50% (−90 to −155 DU (Dobson Unit)) in 1989–1992, and then stayed at around −48% (−160 DU). The ozone loss in the warmer winters (e.g. 2002 and 2004) is lower (−37 to −46%), and in the very cold winters (e.g. 2003 and 2006) it is higher (−52 to −55%). These loss estimates are in good agreement with those estimated from satellite observations, where the differences are less than ±3%. The ozone trends based on the equivalent effective Antarctic stratospheric chlorine (EEASC) and piecewise linear trend (PWLT) functions for the vortex averaged ground-based, Total Ozone Mapping Spectrometer/Ozone Monitoring Instrument (TOMS/OMI), and MSR data averaged over September–November exhibit about −4.6 DU yr−1 over 1979–1999, corroborating the role of halogens in the ozone decrease during the period. The ozone trends computed for the 2000–2010 period are about +1 DU yr−1 for EEASC and +2.6 DU yr−1 for the PWLT functions. The larger positive PWLT trends for the 2000–2010 period indicate the influence of dynamics and other basis functions on the increase of ozone. The trends in both periods are significant at 95% confidence intervals for all analyses. Therefore, our study suggests that Antarctic ozone shows a significant positive trend toward its recovery, and hence, leaves a clear signature of the successful implementation of the Montreal Protocol.

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 54–71°N and 64–88°S, 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. Considering the accuracy of the other data used for this comparative study, the version 1.4 ozone data are suitably used for quantitative analyses in the high-latitude stratosphere in both the Northern and Southern Hemisphere and in the lower mesosphere in the Southern Hemisphere

Abstract. During a 2-week intercomparison of ground-based zenith sky visible spectrometers in September 1994 at Camborne, United Kingdom (50øN, 5øW), ozone profiles were measured by electrochemical cell (ECC) sondes during 11 twilight periods. We use these profiles and a radiative transfer model to calculate separate air mass factors (AMFs) for each twilight period. We examine ozone data from one of the spectrometers of the Syst•me d'Analyse par Observation Zenithale (SAOZ) design and we show that these separate AMFs give very straight Langley plots, except at solar zenith angles exceeding 90 ø. Total ozone calculated using these AMFs, by a variety of commonly used procedures, agrees with the total ozone calculated by vertically integrating the sonde profiles, with mean differences of 0 to 7 Dobson units (DU), depending on the method, and standard deviations of 9 to 11 DU (1 {•). Total ozone calculated using the best procedure (i.e., averaging twilight values), which is not sensitive to errors in the gradients of AMFs, gave excellent agreement whether using separate AMFs or fixed climatological AMFs. We analyse the variance of the data set and several sources of systematic error in the measurements. We also illustrate from an example during the campaign that such analyses are pointless in the presence of a strong jet stream, which can give rise to changes in ozone during the course of the day that are large enough to invalidate the Langley plot.

Measurements of trace gases and photolysis rates in the troposphere are essential for understanding photochemical smog and global environmental change. Chemical measurement techniques have progressed enormously since the first regular observations of tropospheric ozone in the 19th century. In contrast, by the 1940s spectroscopic measurements were already of a quality that would have allowed the use of modern analysis techniques to reduce interference between gases, although such techniques were not applied at the time. Today, chemical and spectroscopic techniques complement each other on a wide range of platforms. The boundaries between spectroscopic techniques will retreat as more Fourier transform spectrometers are used at visible wavelengths and as wide-band lidars are extended, and combining chemical techniques will allow detection of more trace gases with better sensitivity. Other future developments will focus on smaller, lighter instruments to take advantage of new platforms such as unmanned aircraft and to improve the effectiveness of urban sampling.