Trend analysis of greenhouse gases over Europe measured by a network of ground-based remote FTIR instruments

in Atmospheric Chemistry and Physics (2008), 8(22), 6719-6727

This paper describes the statistical analysis of annual trends in long term datasets of greenhouse gas measurements taken over ten or more years. The analysis technique employs a bootstrap resampling ... [more ▼]

This paper describes the statistical analysis of annual trends in long term datasets of greenhouse gas measurements taken over ten or more years. The analysis technique employs a bootstrap resampling method to determine both the long-term and intra-annual variability of the datasets, together with the uncertainties on the trend values. The method has been applied to data from a European network of ground-based solar FTIR instruments to determine the trends in the tropospheric, stratospheric and total columns of ozone, nitrous oxide, carbon monoxide, methane, ethane and HCFC-22. The suitability of the method has been demonstrated through statistical validation of the technique, and comparison with ground-based in-situ measurements and 3-D atmospheric models. [less ▲]

Satellite validation of column-averaged methane on global scale: ground-based data from 15 FTIR stations versus last generation ENVISAT/SCIAMACHY retrievals

Poster (2008, September)

Previous work has shown that the precision of ground-based mid-infrared (MIR) FTIR spectrometry is sufficient to detect day-to-day variability of columnar methane, while first retrievals from ENVISAT ... [more ▼]

Previous work has shown that the precision of ground-based mid-infrared (MIR) FTIR spectrometry is sufficient to detect day-to-day variability of columnar methane, while first retrievals from ENVISAT/SCIAMACHY (channel 8) satellite measurements were impacted by a significant time-dependent bias due to detector icing. This prevented insight into true methane temporal variability at that time. The goal of our updated study is to investigate the precision of the last generation (channel 6) SCIAMACHY retrievals IMAP-DOAS v49 and WFM-DOAS v1.0 in comparison to retrievals from ground-based MIR measurements of the European FTIR network. We first briefly discuss the origin and magnitude of the natural variability of columnar methane. Subsequently, our study investigates all factors which can be optimized to improve precision of ground-based MIR-FTIR retrievals of columnar methane. This includes an optimized Tikhonov-type regularization tuned in a way to minimize the diurnal variability of retrieved columnar methane. We also discuss ways to select and average individual-pixel satellite data in order to reflect true day-to-day variability and make them comparable to ground-based data. [less ▲]

Validation of MIPAS ClONO2 measurements

in Atmospheric Chemistry and Physics (2007), 7

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 ... [more ▼]

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. [less ▲]

Advanced exploitation of ground-based Fourier transform infrared observations for tropospheric studies over Europe: achievements of the UFTIR project

in Geophysical Research Abstracts (2006), 8

Solar absorption measurements using Fourier transform infrared (FTIR) spectrometry carry information about the atmospheric abundances of many constituents, including information about their vertical ... [more ▼]

Solar absorption measurements using Fourier transform infrared (FTIR) spectrometry carry information about the atmospheric abundances of many constituents, including information about their vertical distributions in the troposphere and the stratosphere. Such observations have regularly been made since many years as a contribution to the NDSC (Network for the Detection of Stratospheric Change). They are the only ground-based remote sensing observations available nowadays that carry information about key atmospheric trace species in the free troposphere, among which the most important greenhouse gases. The European UFTIR project (Time series of Upper Free Troposphere observations from a European ground-based FTIR network, http://www.nilu.no/uftir) has focused on maximizing the information content of FTIR long-term monitoring data of some direct and indirect greenhouse gases (CH4, N2O, O3,HCFC-22, and CO and C2H6, respectively). The UFTIR network includes six NDSC stations in Western Europe, covering the polar to subtropical regions. At several stations of the network, the observations span more than a decade. Existing spectral time series have been reanalyzed according to a common optimized retrieval strategy, in order to derive distinct tropospheric and stratospheric abundances of the abovementioned target gases. A bootstrap resampling method has been implemented to evaluate trends of the tropospheric and total burdens of the target gases, including their uncertainties. In parallel, simulations of the target time series have been made with the Oslo CTM2 model: comparisons between the model results and the observations provide valuable information to improve the model, and in particular, to optimize emission estimates that are used as inputs to the model simulations, and to explain the observed trends. The final results of the project will be presented, and ways to proceed will be discussed. [less ▲]

The exploitation of ground-based Fourier transform infrared observations for the evaluation of tropospheric trends of greenhouse gases over Europe

in Environmental Sciences (2005), 2(2-3), 283-293

Solar absorption measurements using Fourier transform infrared (FTIR) spectrometry carry information about the atmospheric abundances of many constituents, including non-CO2 greenhouse gases. Such ... [more ▼]

Solar absorption measurements using Fourier transform infrared (FTIR) spectrometry carry information about the atmospheric abundances of many constituents, including non-CO2 greenhouse gases. Such observations have regularly been made for many years as a contribution to the Network for the Detection of Stratospheric Change (NDSC). They are the only ground-based remote sensing observations available nowadays that carry information about a number of greenhouse gases in the free troposphere. This work focuses on the discussion of the information content of FTIR long-term monitoring data of some direct and indirect greenhouse gases (CH4, N2O, O3 and CO and C2H6, respectively), at six NDSC stations in Western Europe. This European FTIR network covers the polar to subtropical regions. At several stations of the network, the observations span more than a decade. Existing spectral time series have been reanalyzed according to a common optimized retrieval strategy, in order to derive distinct tropospheric and stratospheric abundances for the above-mentioned target gases. A bootstrap resampling method has been implemented to evaluate trends of the tropospheric burdens of the target gases, including their uncertainties. In parallel, simulations of the target time series are being made with the Oslo CTM2 model: comparisons between the model results and the observations provide valuable information to improve the model and, in particular, to optimize emission estimates that are used as inputs to the model simulations. The work is being performed within the EC project UFTIR. The paper focuses on N2O for which the first trend results have been obtained. [less ▲]

On the use of HF as a reference for the comparison of stratospheric observations and models

in Journal of Geophysical Research (1997), 102(11D), 12901-12919

Hydrogen fluoride (HF) is often used as a simple reference for other column observations of chemically active stratospheric species. However, seasonal and shorter timescale variations in column HF make ... [more ▼]

Hydrogen fluoride (HF) is often used as a simple reference for other column observations of chemically active stratospheric species. However, seasonal and shorter timescale variations in column HF make its use as a reference more complicated. In this paper we characterize the expected magnitude of these variations in HF, and variations of ratio quantities involving HF, using a two-dimensional (2-D) photochemical model and two versions of a three-dimensional (3-D) transport model. The 2-D model predicts that the column ratios HNO3/HF and HCl/HF increase from midlatitudes to the tropics, although this is very sensitive to HCl and HNO3 abundances in the tropical upper troposphere. Seasonal variations in vertical motion modifys the predicted ratios; for example, wintertime descent at high latitudes decreases HCl/HF. The ratio HNO3/HF at high latitudes is strongly modified by seasonal variations in the chemical partitioning of the odd nitrogen (NOy) species. We compare these model predictions with ground-based Fourier transform infrared spectroscopy (FTIR) observations of HF along with HCl, ClONO2 and HNO3 obtained at eight northern hemisphere sites between October 1994 and July 1995. We investigate quantitatively how HF can be used as a tracer to follow the evolution of observations at a single station and to intercompare results from different stations or with photochemical models. The magnitude of the 3-D model HF column agrees well with the observations, except on some occasions at high latitudes, giving indirect support for the important role of COF2 in the stratospheric inorganic fluorine budget. The observed day-to-day variability in the column ratios HCl/HF and HNO3/HF is much larger at high latitudes. This variability is reproduced in the 3-D models and is due to horizontal motion. Short timescale vertical displacement of the species profiles is estimated to have a small effect on the column ratios. In particular, we analyze the usefulness of the observed column ratio (ClONO2 + HCl)/HF as an indicator for chlorine activation. Current measurement uncertainties limit the degree of activation which can be unambiguously detected using this observed quantity, but we can determine that chlorine-activated air was observed above Aberdeen (58 degrees N) on 6 days in late January 1995. [less ▲]