Abstract. Within the project MUSICA (MUlti-platform remote Sensing of Isotopologues for investigating the Cycle of Atmospheric water) ground-and space-based remote sensing as well as in situ data sets of tropospheric water vapour isotopologues are provided. The space-based remote-sensing data set is produced from spectra measured by the IASI (Infrared Atmospheric Sounding Interferometer) sensor and is potentially available on a global scale.Here, we present the MUSICA IASI data for three different geophysical locations (subtropics, midlatitudes, and Arctic), and we provide a comprehensive characterisation of the complex nature of such space-based isotopologue remotesensing products. The quality assessment study is complemented by a comparison to MUSICA's ground-based FTIR (Fourier Transform InfraRed) remote-sensing data retrieved from the spectra recorded at three different locations within the framework of NDACC (Network for the Detection of Atmospheric Composition Change).We confirm that IASI is able to measure tropospheric H 2 O profiles with a vertical resolution of about 4 km and a random error of about 10 %. In addition IASI can observe middle tropospheric δD that adds complementary value to IASI's middle tropospheric H 2 O observations. Our study presents theoretical and empirical proof that IASI has the capability for a global observation of middle tropospheric water vapour isotopologues on a daily timescale and at a quality that is sufficiently high for water cycle research purposes.

Abstract. We compare measurements of integrated water vapour (IWV) over a subarctic site (Kiruna, Northern Sweden) from five different sensors and retrieval methods: Radiosondes, Global Positioning System (GPS), ground-based Fourier-transform infrared (FTIR) spectrometer, groundbased microwave radiometer, and satellite-based microwave radiometer (AMSU-B). Additionally, we compare also to ERA-Interim model reanalysis data. GPS-based IWV data have the highest temporal coverage and resolution and are chosen as reference data set. All datasets agree reasonably well, but the ground-based microwave instrument only if the data are cloud-filtered. We also address two issues that are general for such intercomparison studies, the impact of different lower altitude limits for the IWV integration, and the impact of representativeness error. We develop methods for correcting for the former, and estimating the random error contribution of the latter. A literature survey reveals that reported systematic differences between different techniques are study-dependent and show no overall consistent pattern. Further improving the absolute accuracy of IWV measurements and providing climate-quality time series therefore remain challenging problems.

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.

Abstract. Trends in the CO and C 2 H 6 partial columns (∼0-15 km) have been estimated from four European groundbased solar FTIR (Fourier Transform InfraRed) stations for the 1996-2006 time period. The CO trends from the four stations Jungfraujoch, Zugspitze, Harestua and Kiruna have been estimated to −0.45 ± 0.16 % yr −1 , −1.00 ± 0.24 % yr −1 , −0.62 ± 0.19 % yr −1 and −0.61 ± 0.16 % yr −1 , respectively. The corresponding trends for C 2 H 6 are −1.51± 0.23 % yr −1 , −2.11 ± 0.30 % yr −1 , −1.09 ± 0.25 % yr −1 and −1.14 ± 0.18 % yr −1 . All trends are presented with their 2-σ confidence intervals. To find possible reasons for the CO trends, the global-scale EMEP MSC-W chemical transport model has been used in a series of sensitivity scenarios. It is shown that the trends are consistent with the combination of a 20 % decrease in the anthropogenic CO emissions seen in Europe and North America during the 1996-2006 period and a 20 % increase in the anthropogenic CO emissions in East Asia, during the same time period. The possible impacts of CH 4 and biogenic volatile organic compounds (BVOCs) are also considered. The European and global-scale EMEP models have been evaluated against the Correspondence to: J. Mellqvist (johan.mellqvist@chalmers.se) measured CO and C 2 H 6 partial columns from Jungfraujoch, Zugspitze, Bremen, Harestua, Kiruna and Ny-Ålesund. The European model reproduces, on average the measurements at the different sites fairly well and within 10-22 % deviation for CO and 14-31 % deviation for C 2 H 6 . Their seasonal amplitude is captured within 6-35 % and 9-124 % for CO and C 2 H 6 , respectively. However, 61-98 % of the CO and C 2 H 6 partial columns in the European model are shown to arise from the boundary conditions, making the globalscale model a more suitable alternative when modeling these two species. In the evaluation of the global model the average partial columns for 2006 are shown to be within 1-9 % and 37-50 % of the measurements for CO and C 2 H 6 , respectively. The global model sensitivity for assumptions made in this paper is also analyzed.

Abstract. This work presents the methane (CH4) and nitrous oxide (N2O) products as generated by the IASI (Infrared Atmospheric Sounding Interferometer) processor developed during the project MUSICA (MUlti-platform remote Sensing of Isotopologues for investigating the Cycle of Atmospheric water). The processor retrieves CH4 and N2O with different water vapour and water vapour isotopologues (as well as HNO3) and uses a single a priori data set for all the retrievals (no variation in space and time). Firstly, the characteristics and errors of the products are analytically described. Secondly, the products are comprehensively evaluated by comparisons to the following reference data measured by different techniques and from different platforms as follows: (1) aircraft CH4 and N2O profiles from the five HIAPER Pole-to-Pole Observation (HIPPO) missions; (2) continuous in situ CH4 and N2O observations performed between 2007 and 2017 at subtropical and mid-latitude high-mountain observatories (Izaña Atmospheric Observatory and Jungfraujoch, respectively) in the framework of the WMO–GAW (World Meteorological Organization–Global Atmosphere Watch) programme; (3) ground-based FTIR (Fourier-transform infrared spectrometer) measurements made between 2007 and 2017 in the framework of the NDACC (Network for the Detection of Atmospheric Composition Change) at the subtropical Izaña Atmospheric Observatory, the mid-latitude station of Karlsruhe and the Kiruna polar site.The theoretical estimations and the comparison studies suggest a precision for the N2O and CH4 retrieval products of about 1.5–3 % and systematic errors due to spectroscopic parameters of about 2 %. The MUSICA IASI CH4 data offer a better sensitivity than N2O data. While for the latter the sensitivity is mainly limited to the UTLS (upper troposphere–lower stratosphere) region, for CH4 we are able to prove that at low latitudes the MUSICA IASI processor can detect variations that take place in the free troposphere independently from the variations in the UTLS region. We demonstrate that the MUSICA IASI data qualitatively capture the CH4 gradients between low and high latitudes and between the Southern Hemisphere and Northern Hemisphere; however, we also find an inconsistency between low- and high-latitude CH4 data of up to 5 %. The N2O latitudinal gradients are very weak and cannot be detected. We make comparisons over a 10-year time period and analyse the agreement with the reference data on different timescales. The MUSICA IASI data can detect day-to-day signals (only in the UTLS), seasonal cycles and long-term evolution (in the UTLS and for CH4 also in the free troposphere) similar to the reference data; however, there are also inconsistencies in the long-term evolution connected to inconsistencies in the used atmospheric temperature a priori data.Moreover, we present a method for analytically describing the a posteriori-calculated logarithmic-scale difference of the CH4 and N2O retrieval estimates. By correcting errors that are common in the CH4 and N2O retrieval products, the a posteriori-calculated difference can be used for generating an a posteriori-corrected CH4 product with a theoretically better precision than the original CH4 retrieval products. We discuss and evaluate two different approaches for such a posteriori corrections. It is shown that the correction removes the inconsistencies between low and high latitudes and enables the detection of day-to-day signals also in the free troposphere. Furthermore, they reduce the impact of short-term atmospheric dynamics, which is an advantage, because respective signals are presumably hardly comparable to model data. The approach that affects the correction solely on the scales on which the errors dominate is identified as the most efficient, because it reduces the inconsistencies and errors without removing measurable real atmospheric signals. We give a brief outlook on a possible usage of this a posteriori-corrected MUSICA IASI CH4 product in combination with inverse modelling.