Trends of CO2, CH4 and N2O over 1985-2010 from high-resolution FTIR solar observations at the Jungfraujoch station

Two state-of-the-art Fourier Transform Infrared (FTIR) spectrometers are operated at the Jungfraujoch station (46.5ºN, 8.0ºE, 3580m asl) within the framework of the Network for the Detection of Atmospheric Composition Change (NDACC, visit http://www.ndacc.org). The earliest FTIR observations have been obtained there in 1984. Since then, regular recordings of high-resolution solar absorption spectra have been performed at that site, under clear-sky conditions, allowing to collect almost 29000 observations relevant to the present communication. We present time series of three greenhouse gases targeted by the Kyoto Protocol: CO2, CH4 (and its isotopologue 13CH4) and N2O. These data sets have been obtained with the SFIT-2 algorithm which implements the Optimal Estimation Method of Rodgers (1990). This allows retrieving total columns of the target gases as well as information on their distribution with altitude. For the methane isotopologues and N2O, a Tikhonov L1 regularization scheme has been applied, as part of an harmonization effort carried out within the European HYMN project (see also Dils et al, 2010; Foster et al., 2010). Trends –and their associated uncertainties– characterizing these long series as well as the seasonal modulations have been determined with a statistical tool using bootstrap resampling (Gardiner et al., 2008). Trend values will be presented and critically discussed; in particular, we will investigate if significant changes in the rate of accumulations of these four atmospheric gases occurred over the last 25 years. Numerous additional greenhouse gases are accessible to the FTIR technique. Examples of such trend studies are reported at the EGU General Assembly by Mahieu et al. (2010) and Rinsland et al. (2010)

Spectroscopic Detection of COClF in the Tropical and Mid-Latitude Lower Stratosphere

We report retrievals of COClF (carbonyl chlorofluoride) based on atmospheric chemistry experiment (ACE) solar occultation spectra recorded at tropical and mid-latitudes during 2004-2005. The COClF molecule is a temporary reservoir of both chlorine and fluorine and has not been measured previously by remote sensing. A maximum COClF mixing ratio of 99.7+/-48.0 pptv (10(exp -12) per unit volume, 1 sigma) is measured at 28km for tropical and subtropical occultations (latitudes below 20deg in both hemispheres) with lower mixing ratios at both higher and lower altitudes. Northern hemisphere mid-latitude mixing ratios (30-50degN) resulted in an average profile with a peak mixing ratio of 51.7+/-32.1 pptv, 1 sigma, at 27 km, also decreasing above and below that altitude. We compare the measured average profiles with the one reported set of in situ lower stratospheric mid-latitude measurements from 1986 and 1987, a previous two-dimensional (2-D) model calculation for 1987 and 1993, and a 2-D-model prediction for 2004. The measured average tropical profile is in close agreement with the model prediction; the northern mid-latitude profile is also consistent, although the peak in the measured profile occurs at a higher altitude (2.5-4.5km offset) than in the model prediction. Seasonal average 2-D-model predictions of the COClF stratospheric distribution for 2004 are also reported

Changes in atmospheric composition discerned from long-term NDACC measurements: trends in direct greenhouse gases derived from infrared solar absorption spectra recorded at the Jungfraujoch station

The University of Liège (ULg) is operating -under clear sky conditions- two state-of-the-art Fourier Transform Infrared (FTIR) spectrometers at the high-altitude research station of the Jungfraujoch (Swiss Alps, 46.5ºN, 3580m asl), within the framework of the Network for the Detection of Atmospheric Composition Changes (NDACC). Routine FTIR operation started in 1984. Since then, it has been continued without disruption, allowing collecting more than 45000 high-resolution broadband IR solar absorption spectra, between 2 and 16 µm, using either HgCdTe or InSb detectors as well as a suite of optical filters. Typically, the spectral resolutions achieved lie in the 0.003 to 0.009 cm-1 interval while signal-to-noise ratios of 1000 and more are reached. Numerous narrow-band IR spectra essentially recorded from 1976 to 1989 with grating instruments are also available. Their analyses with modern tools have recently started [Bader et al., 2011] and will be pursued to consistently extend our datasets back in the 1970s. Geophysical parameters are deduced from the ULg observational database either with the SFIT-1, SFIT-2 or PROFFIT-9 algorithm, allowing producing total column time series of the target gases. In addition, information on their vertical distributions with altitude can generally be derived when using SFIT-2 or PROFFIT-9 which both implement the Optimal Estimation Method of Rodgers [1990]. Presently, more than two dozen atmospheric species are systematically retrieved from the Jungfraujoch observations, allowing the monitoring of key constituents of the Earth's atmosphere which play important roles in stratospheric ozone depletion and/or in global warming. This communication will focus on the direct and major greenhouse gases available from our database, namely water vapor, CO2, CH4, N2O, tropospheric ozone, CFC-11, CFC-12, HCFC-22, CCl4, SF6, as well as CF4 which has recently been added to our targets list [Duchatelet et al., 2011]. Trends and associated uncertainties characterizing the available -and often multi-decadal- time series have been derived or updated with a statistical bootstrap resampling tool [Gardiner et al., 2008], they will be presented and critically compared with data available from the literature

Validation of MIPAS ClONO2 measurements

Altitude profiles of ClONO2 retrieved with the IMK (Institut fur Meteorologie und Klimaforschung) science-oriented data processor from MIPAS/Envisat (Michelson Interferometer for Passive Atmospheric Sounding on Envisat) mid-infrared limb emission measurements between July 2002 and March 2004 have been validated by comparison with balloon-borne (Mark IV, FIRS2, MIPAS-B), airborne (MIPAS-STR), ground-based (Spitsbergen, Thule, Kiruna, Harestua, Jungfraujoch, Izana, Wollongong, Lauder), and spaceborne (ACE-FTS) observations. With few exceptions we found very good agreement between these instruments and MIPAS with no evidence for any bias in most cases and altitude regions. For balloon-borne measurements typical absolute mean differences are below 0.05 ppbv over the whole altitude range from 10 to 39 km. In case of ACE-FTS observations mean differences are below 0.03 ppbv for observations below 26 km. Above this altitude the comparison with ACE-FTS is affected by the photochemically induced diurnal variation of ClONO2. Correction for this by use of a chemical transport model led to an overcompensation of the photochemical effect by up to 0.1 ppbv at altitudes of 30-35 km in case of MIPAS-ACE-FTS comparisons while for the balloon-borne observations no such inconsistency has been detected. The comparison of MIPAS derived total column amounts with ground-based observations revealed no significant bias in the MIPAS data. Mean differences between MIPAS and FTIR column abundances are 0.11 +/- 0.12 x 10(14) cm(-2) (1.0 +/- 1.1%) and -0.09 +/- 0.19 x 10(14) cm(-2) (-0.8 +/- 1.7%), depending on the coincidence criterion applied. chi(2) tests have been performed to assess the combined precision estimates of MIPAS and the related instruments. When no exact coincidences were available as in case of MIPAS-FTIR or MIPAS-ACE-FTS comparisons it has been necessary to take into consideration a coincidence error term to account for chi(2) deviations. From the resulting chi(2) profiles there is no evidence for a systematic over/underestimation of the MIPAS random error analysis.Peer reviewe

Observations, par ballon stratosphériques, du spectre solaire à 1.85 microns avec un pouvoir de resolution de 135.000

Le 6 avril 1970, l'Institut d'Astrophysique de l'Université de Liège a lancé une nacelle stratosphérique transportant un télescope de 40 cm d'ouverture et un spectromètre à réseau du type Ebert-Fastie, de 2,50 m de focale. Les spectres solaires obtenus dans la bande de H2O, centrée à 1,87 microns, avec une résolution spectrale de .04 cm-1, ont permis de déterminer avec grande précision plus de 60 raies solaires pour la plupart non encore identifiées, entre 5480.0 et 5382 cm-1. L'étude de raies d'absorption dues à la vapeur d'eau tellurique indique que la stratosphère est sèche, avec un taux de mélange moyen de l'ordre de 2 X 10-6gg-1 ; la possibilité d'une augmentation du taux de mélange au-dessus de 40 km d'altitude n'est pas à exclure au stade actuel de l'exploitation des données.Zander R. Observations, par ballon stratosphérique, du spectre solaire à 1,85 microns avec un pouvoir de résolution de 135.000. In: Bulletin de la Classe des sciences, tome 56, 1970. pp. 729-739

Présence de HF dans la stratosphere supérieure

peer reviewedDes observations solaires effectuées par ballon à 27,5 km d'altitude ont permis d'enregistrer le spectre du Soleil au voisinage de 2,5 μ, avec une résolution égale à 0.04 cm-1. Une raie d'absorption observée à 4038,97 cm-1 a été attribuée à HF qui serait présent dans la stratosphère supérieure.Solar observations performed with a stratospheric gondola at 27.5 km altitude have allowed recording the solar spectrum near 2.5 μ, with a resolution of 0.04 cm-1. An absorption line observed at 4038.97 cm-1 has been attributed to HF, a species which would be present in the upper stratosphere