Observation of unusual chlorine activation by ground-based infrared and microwave spectroscopy in the late Arctic winter 2000/01

International audienceDuring the Arctic winter of 2000/01, ground-based FTIR and millimetre-wave measurements revealed significant amounts of ClO over Kiruna after the final warming in February 2001. In fact, column amounts of ClO were still increased in March 2001 when temperatures were about 20K above the PSC (Polar Stratospheric Clouds) threshold. At these temperatures, chlorine activation due to heterogeneous processes on PSCs is not possible even in the presence of strong lee wave effects. In order to discuss possible reasons of this feature, time series of other chemical species will be presented and discussed, too. Measurements of HF and COF2 indicated that vortex air was still observed in mid-March 2001. Since the time series of HNO3 column amounts do not give any evidence of a denitrification later than 11 February, chlorine activation persisting for several weeks after the presence of PSCs due to denitrification is rather unlikely. The photolysis of ClONO2-rich air which had been formed at the end of February and beginning of March 2001 as well as chlorine activation due to the presence of an unusual aerosol layer are discussed as possible causes of the increased ClO column amounts after the final warming

Trends of HCl, ClONO₂, and HF column abundances from ground-based FTIR measurements in Kiruna (Sweden) in comparison with KASIMA model calculations

Trends of hydrogen chloride (HCl), chlorine nitrate (ClONO2), and hydrogen fluoride (HF) total column abundances above Kiruna (Northern Sweden, 67.84$^\circ\text{N}$, 20.41$^\circ\text{E}$) derived from nearly 14 years (1996–2009) of measurement and model data are presented. The measurements have been performed with a Bruker 120HR (later Bruker 125 HR) Fourier transform infrared (FTIR) spectrometer and the chemistry-transport model (CTM) used was KASIMA (KArlsruhe SImulation model of the Middle Atmosphere). The total column abundances of ClONO2 and HF calculated by KASIMA agree quite well with the FTIR measurements while KASIMA tends to underestimate the HCl columns. To calculate the long-term trends, a linear function combined with an annual cycle was fitted to the data using a least squares method. The precision of the resulting trends was estimated with the bootstrap resampling method. For HF, both model and measurements show a positive trend that seems to decrease in the last few years. This suggests a stabilisation of the HF total column abundance. Between 1996 and 2009, KASIMA simulates an increase of (+1.51±0.07) %/yr which exceeds the FTIR result of (+0.65±0.25) %/yr. The trends determined for HCl and ClONO2 are significantly negative over the time period considered here. This is expected because the emission of their precursors (chlorofluorocarbons and hydrochlorofluorocarbons) has been restricted in the Montreal Protocol in 1987 and its amendments and adjustments. The trend for ClONO2 from the FTIR measurements amounts to (−3.28±0.56)%/yr and the one for HCl to (−0.81±0.23)%/yr. KASIMA simulates a weaker decrease: For ClONO2, the result is (−0.90±0.10) %/yr and for HCl (−0.17±0.06) %/yr. Part of the difference between measurement and model data can be explained by sampling and the stronger annual cycle indicated by the measurements. There is a factor of about four between the trends of HCl and ClONO2 above Kiruna for both measurement and model data

A multi-instrument comparison of integrated water vapour measurements at a high latitude site

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

Lunar and solar FTIR nitric acid measurements at Eureka in winter 2001/2002: comparisons with observations at Thule and Kiruna and with CMAM and SLIMCAT model calculations

For the first time, vertical column measurements of (HNO3) above the Arctic Stratospheric Ozone Observatory (AStrO) at Eureka (80N, 86W), Canada, have been made during polar night using lunar spectra recorded with a Fourier Transform Infrared (FTIR) spectrometer, from October 2001 to March 2002. AStrO is part of the primary Arctic station of the Network for the Detection of Stratospheric Change (NDSC). These measurements were compared with FTIR measurements at two other NDSC Arctic sites: Thule, Greenland (76.5N, 68.8W) and Kiruna, Sweden (67.8N, 20.4E). The measurements were also compared with two atmospheric models: the Canadian Middle Atmosphere Model (CMAM) and SLIMCAT. This is the first time that CMAM HNO3 columns have been compared with observations in the Arctic. Eureka lunar measurements are in good agreement with solar ones made with the same instrument. Eureka and Thule HNO3 columns are consistent within measurement error. Differences among HNO3 columns measured at Kiruna and those measured at Eureka and Thule can be explained on the basis of the available sunlight hours and the polar vortex location. The comparison of CMAM HNO3 columns with Eureka and Kiruna data shows good agreement, considering CMAM small inter-annual variability. The warm 2001/02 winter with almost no Polar Stratospheric Clouds (PSCs) makes the comparison of the warm climate version of CMAM with these observations a good test for CMAM under no PSC conditions. SLIMCAT captures the magnitude of HNO3 columns at Eureka, and the day-to-day variability, but generally reports higher HNO3 columns than the CMAM climatological mean columns

The MUSICA IASI CH4 and N2O products and their comparison to HIPPO, GAW and NDACC FTIR references

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.This work has strongly benefited from funding by the European Research Council under FP7/(2007–2013)/ERC grant agreement no. 256961 (project MUSICA); by the Deutsche Forschungsgemeinschaft for the project MOTIV (Geschäftszeichen SCHN 1126/2-1); by the Ministerio de Economía y Competitividad from Spain trough the projects CGL2012-37505 (project NOVIA) and CGL2016-80688-P (project INMENSE); by the Ministerio de Educación, Cultura y Deporte (programa “José Castillejo”, CAS14/00282); and by EUMETSAT under its Fellowship Programme (project VALIASI)

Carbon monoxide (CO) and ethane (C₂H₆) trends from ground-based solar FTIR measurements at six European stations, comparison and sensitivity analysis with the EMEP model

Trends in the CO and C2H6 partial columns (~0–15 km) have been estimated from four European groundbasedsolar 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 C2H6 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 CH4 and biogenic volatile organic compounds (BVOCs) are also considered. The European and global-scale EMEP models have been evaluated against the measured CO and C2H6 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 C2H6. Their seasonal amplitude is captured within 6–35% and 9–124% for CO and C2H6, respectively. However, 61–98% of the CO and C2H6 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 C2H6, respectively. The global model sensitivity for assumptions made in this paper is also analyzed

The MUSICA MetOp/IASI H2O and deltaD products: characterisation and long-term comparison to NDACC/FTIR data

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 remote-sensing products. The quality assessment study is complemented by a comparison to MUSICA\u27s 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 H2O 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\u27s middle tropospheric H2O 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