The FTIR and MAX-DOAS daily mean total columns agree very well: no significant bias is observed and the standard deviation of the comparisons is only 8%. Both FTIR and MAX-DOAS HCHO total columns are in good agreement with SCIAMACHY values in the 2004-2005 period, with standard deviations of 21% and 31%, respectively. The same seasonal cycle is observed by the different instruments, with a minimum in austral winter and a maximum in FebruaryMarch.The FTIR and MAX-DOAS data are confronted with HCHO columns calculated by a global CTM, the IMAGES model. The model underestimates the HCHO columns by 23-29% in comparison with FTIR, and by 15% in comparison with DOAS. This bias might have multiple causes, including an underestimation of OH concentrations in the model (as indicated by a sensitivity study using prescribedCorrespondence to: C. Vigouroux (corinne.vigouroux@aeronomie.be) OH fields) and/or an underestimated contribution of largescale transport of HCHO precursors from Madagascar. The latter hypothesis is comforted by the large observed day-today variability of HCHO columns, and by the observation that the peak values of FTIR columns can often be associated with free tropospheric transport patterns from source regions over Madagascar to Réunion Island, according to simulations performed with the Lagrangian particle dispersion model FLEXPART.

International audienceWe show carbon monoxide (CO) distributions at different vertical levels over the subtropical southern Indian Ocean, analyzing an observation campaign using Fourier transform infrared (FTIR) solar absorption spectrometry performed in 2007 at Reunion Island (21°S, 55°E). The CO pollution levels detected by the FTIR measurements during the campaign show a doubling of the CO total columns during the Southern Hemisphere biomass burning season. Using correlative data from the Measurement of Pollution in the Troposphere instrument and back trajectories analyses, we show that the potential primary sources for CO throughout the troposphere in 2007 are southern Africa (June-August) and South America (September-October). A secondary potential contribution from Southeast Asia and Indonesia-Malaysia was identified in the upper troposphere, especially in July and September. We examine the relation between the Asian monsoon anticyclone seasonal cycle and this result. We also investigate the relative contribution of different areas across the globe to the CO concentration in the subtropical southern Indian Ocean in 2007 using backward simulations combining the Lagrangian model FLEXPART 6.2, the Global Fire Emissions Database (GFEDv2.1) and the Emission Database for Global Atmospheric Research (EDGARv3.2-FT2000). We confirm the predominance of the African and South American contributions in the CO concentration in the southern subtropical Indian Ocean below 11 km. We show that CO transported from Australia makes only a small contribution to the total CO concentration observed over Reunion Island, and that the long-range transport of CO coming from Southeast Asia and Indonesia-Malaysia is important, especially from June until September in the upper troposphere

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Abstract. Time series of total column abundances of hydrogen chloride (HCl), chlorine nitrate (ClONO2), and hydrogen fluoride (HF) were determined from ground-based Fourier transform infrared (FTIR) spectra recorded at 17 sites belonging to the Network for the Detection of Atmospheric Composition Change (NDACC) and located between 80.05° N and 77.82° S. By providing such a near-global overview on ground-based measurements of the two major stratospheric chlorine reservoir species, HCl and ClONO2, the present study is able to confirm the decrease of the atmospheric inorganic chlorine abundance during the last few years. This decrease is expected following the 1987 Montreal Protocol and its amendments and adjustments, where restrictions and a subsequent phase-out of the prominent anthropogenic chlorine source gases (solvents, chlorofluorocarbons) were agreed upon to enable a stabilisation and recovery of the stratospheric ozone layer. The atmospheric fluorine content is expected to be influenced by the Montreal Protocol, too, because most of the banned anthropogenic gases also represent important fluorine sources. But many of the substitutes to the banned gases also contain fluorine so that the HF total column abundance is expected to have continued to increase during the last few years. The measurements are compared with calculations from five different models: the two-dimensional Bremen model, the two chemistry-transport models KASIMA and SLIMCAT, and the two chemistry-climate models EMAC and SOCOL. Thereby, the ability of the models to reproduce the absolute total column amounts, the seasonal cycles, and the temporal evolution found in the FTIR measurements is investigated and inter-compared. This is especially interesting because the models have different architectures. The overall agreement between the measurements and models for the total column abundances and the seasonal cycles is good. Linear trends of HCl, ClONO2, and HF are calculated from both measurement and model time series data, with a focus on the time range 2000–2009. This period is chosen because from most of the measurement sites taking part in this study, data are available during these years. The precision of the trends is estimated with the bootstrap resampling method. The sensitivity of the trend results with respect to the fitting function, the time of year chosen and time series length is investigated, as well as a bias due to the irregular sampling of the measurements. The measurements and model results investigated here agree qualitatively on a decrease of the chlorine species by around 1% yr−1. The models simulate an increase of HF of around 1% yr−1. This also agrees well with most of the measurements, but some of the FTIR series in the Northern Hemisphere show a stabilisation or even a decrease in the last few years. In general, for all three gases, the measured trends vary more strongly with latitude and hemisphere than the modelled trends. Relative to the FTIR measurements, the models tend to underestimate the decreasing chlorine trends and to overestimate the fluorine increase in the Northern Hemisphere. At most sites, the models simulate a stronger decrease of ClONO2 than of HCl. In the FTIR measurements, this difference between the trends of HCl and ClONO2 depends strongly on latitude, especially in the Northern Hemisphere.