New multi-station and multi-decadal trend data on precipitable water. Recipe to match FTIR retrievals from NDACC long-time records to radio sondes within 1mm accuracy/precision

in Geophysical Research Abstracts (2009), 11

We present an original optimum strategy for retrieval of precipitable water from routine ground-based midinfrared FTS measurements performed at a number globally distributed stations within the NDACC ... [more ▼]

We present an original optimum strategy for retrieval of precipitable water from routine ground-based midinfrared FTS measurements performed at a number globally distributed stations within the NDACC network. The strategy utilizes FTIR retrievals which are set in a way to match standard radio sonde operations. Thereby, an unprecedented accuracy and precision for measurements of precipitable water can be demonstrated: the correlation between Zugspitze FTIR water vapor columns from a 3 months measurement campaign with total columns derived from coincident radio sondes shows a regression coefficient of R = 0.988, a bias of 0.05 mm, a standard deviation of 0.28 mm, an intercept of 0.01 mm, and a slope of 1.01. This appears to be even better than what can be achieved with state-of-the-art micro wave techniques, see e.g., Morland et al. (2006, Fig. 9 therein). Our approach is based upon a careful selection of spectral micro windows, comprising a set of both weak and strong water vapor absorption lines between 839.4 – 840.6 cm-1, 849.0 – 850.2 cm-1, and 852.0 – 853.1 cm-1, which is not contaminated by interfering absorptions of any other trace gases. From existing spectroscopic line lists, a careful selection of the best available parameter set was performed, leading to nearly perfect spectral fits without significant forward model parameter errors. To set up the FTIR water vapor profile inversion, a set of FTIR measurements and coincident radio sondes has been utilized. To eliminate/minimize mismatch in time and space, the Tobin best estimate of the state of the atmosphere principle has been applied to the radio sondes. This concept uses pairs of radio sondes launched with a 1-hour separation, and derives the gradient from the two radio sonde measurements, in order to construct a virtual PTU profile for a certain time and location. Coincident FTIR measurements of water vapor columns (two hour mean values) have then been matched to the water columns obtained by integrating the best-estimate radio sonde profiles. This match was achieved via investigating the quality of the correlation plots between the columns derived from the radio sondes and the FTIR retrievals, and iteratively tuning the regularization strength of the FTIR retrieval. The FTIR regularization matrix is based on a Tikhonov operator which allows for empirical tuning of the regularization strength via one parameter. The figures of merit for the iterative tuning have been the slope, the intercept, and the regression coefficient of the correlation. By this way an optimum retrieval setting could be found, guaranteeing a response of the FTIR retrievals to true water vapor changes, which is matched to the radio sonde operation. As first examples for utilizing this approach to derive long-term trends of precipitable water from NDACC type long-term FTIR measurements, we present trends from two time series. I.e., one retrieved from continuous FTIR measurements at the NDACC Primary Station Zugspitze, Germany (47.42 °N, 10.98 °E, 2964 m a.s.l.), which covers the time span 1995-2009, and one from the International Scientific Station of the Jungfraujoch (ISSJ, 46.5°N, 8.0°E, 3580m a.s.l., Swiss Alps), covering the time span 1984 – 2009. A detailed trend analysis of both series via the bootstrap method will be presented. In ongoing work we apply this optimum retrieval approach to historical long-time measurement series of further selected FTIR stations of the NDACC network. Thereby we will obtain unprecedented new climate data via long term trends of precipitable water at a set of globally distributed locations. [less ▲]

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 ▲]

Validation of SCIAMACHY CH4 scientific products using ground-based FTIR measurements

Poster (2008, September)

In the framework of the past EVERGREEN project, the development of three scientific algorithms, namely WFM-DOAS (henceforward called WFMD), IMAP-DOAS (henceforward called IMAP) and IMLM, commenced in ... [more ▼]

In the framework of the past EVERGREEN project, the development of three scientific algorithms, namely WFM-DOAS (henceforward called WFMD), IMAP-DOAS (henceforward called IMAP) and IMLM, commenced in order to retrieve the total column amounts of key atmospheric trace gases, including CH4, from SCIAMACHY nadir observations in its near-infrared channels. Since then, the retrieval products of these three algorithms, have undergone serious improvements. At key phases in their development, the products have been validated by using a network of ground-based FTIR instruments. Parallel with the improved SCIAMACHY data, the FTIR groups have taken steps to optimise and harmonise their own datasets and as such the different validation efforts always used the state-of-the-art FTIR dataset. Here we present an overview of the evolution of the CH4 algorithms by re-validating the data, using the same FTIR dataset (as developed under the UFTIR project) for all algorithm versions. [less ▲]

Validation of ACE-FTS N2O measurements

in Atmospheric Chemistry and Physics (2008), 8(16), 4759-4786

The Atmospheric Chemistry Experiment (ACE), also known as SCISAT, was launched on 12 August 2003, carrying two instruments that measure vertical profiles of atmospheric constituents using the solar ... [more ▼]

The Atmospheric Chemistry Experiment (ACE), also known as SCISAT, was launched on 12 August 2003, carrying two instruments that measure vertical profiles of atmospheric constituents using the solar occultation technique. One of these instruments, the ACE Fourier Transform Spectrometer (ACE-FTS), is measuring volume mixing ratio (VMR) profiles of nitrous oxide (N2O) from the upper troposphere to the lower mesosphere at a vertical resolution of about 3-4 km. In this study, the quality of the ACE-FTS version 2.2 N2O data is assessed through comparisons with coincident measurements made by other satellite, balloon-borne, aircraft, and ground-based instruments. These consist of vertical profile comparisons with the SMR, MLS, and MIPAS satellite instruments, multiple aircraft flights of ASUR, and single balloon flights of SPIRALE and FIRS-2, and partial column comparisons with a network of ground-based Fourier Transform InfraRed spectrometers (FTIRs). Between 6 and 30 km, the mean absolute differences for the satellite comparisons lie between -42 ppbv and +17 ppbv, with most within +/- 20 ppbv. This corresponds to relative deviations from the mean that are within +/- 15%, except for comparisons with MIPAS near 30 km, for which they are as large as 22.5%. Between 18 and 30 km, the mean absolute differences for the satellite comparisons are generally within +/- 10 ppbv. From 30 to 60 km, the mean absolute differences are within +/- 4 ppbv, and are mostly between -2 and +1 ppbv. Given the small N2O VMR in this region, the relative deviations from the mean are therefore large at these altitudes, with most suggesting a negative bias in the ACE-FTS data between 30 and 50 km. In the comparisons with the FTIRs, the mean relative differences between the ACE-FTS and FTIR partial columns (which cover a mean altitude range of 14 to 27 km) are within +/- 5.6% for eleven of the twelve contributing stations. This mean relative difference is negative at ten stations, suggesting a small negative bias in the ACE-FTS partial columns over the altitude regions compared. Excellent correlation (R=0.964) is observed between the ACE-FTS and FTIR partial columns, with a slope of 1.01 and an intercept of -0.20 on the line fitted to the data. [less ▲]

Impact of different spectroscopic datasets on CH4 retrievals from Jungfraujoch FTIR spectra

Poster (2008, August)

Methane (CH4) is released in the atmosphere by natural processes (e.g. wetlands, termites) as well as by anthropogenic activities (e.g. fossil fuel exploitation, rice agriculture, biomass burning, etc ... [more ▼]

Methane (CH4) is released in the atmosphere by natural processes (e.g. wetlands, termites) as well as by anthropogenic activities (e.g. fossil fuel exploitation, rice agriculture, biomass burning, etc). Due to its high warming potential and its relatively long chemical lifetime (~9 years), atmospheric methane plays a major role in the radiative forcing responsible of the greenhouse effect. Methane also affects climate by influencing tropospheric ozone and stratospheric water. The cycle of methane is complex and to understand it requires a complete study of its emissions and its budget of sources and sinks. High quality methane data sets are needed to perform such studies. CH4 vertical distributions as well as total and partial column time series can be retrieved from high-resolution ground-based FTIR spectra, using, e.g., the SFIT-2 algorithm which implements the Optimal Estimation Method of Rodgers. A set of 5 microwindows - located in the 2 to 5.5 µm range and jointly adopted by all partners involved in the European HYMN project (www.knmi.nl/samenw/hymn/) - are fitted simultaneously during the retrieval procedure. Although this approach provides relatively high information content, CH4 retrieved profiles very often present large oscillations in the troposphere, which might result partly from inappropriate or inconsistent spectroscopic parameters. Significant improvements on retrieval quality could be reached by using more accurate CH4 spectroscopic parameters. This contribution compares 3 different sets of CH4 spectroscopic parameters (including HITRAN 2004 and 2 versions where HITRAN 2004 have been updated by recent laboratory measurements), which have been tested using one year of high resolution FTIR solar observations performed at the International Scientific Station of the Jungfraujoch (Swiss Alps, 46.5°N, 8.0 °E, 3580m a.s.l.). The impact of these different spectroscopic datasets on retrieved CH4 partial columns and vertical profiles, as well as on the fitting quality (residuals) and on the error budget characterizing our CH4 products will be evaluated and discussed. [less ▲]

Our Changing Atmosphere: Evidence Based on Long-Term Infrared Solar Observations at the Jungfraujoch since 1950

in Science of the Total Environment (2008), 391(2-3), 184-95

The Institute of Astrophysics of the University of Liege has been present at the High Altitude Research Station Jungfraujoch, Switzerland, since the late 1940s, to perform spectrometric solar observations ... [more ▼]

The Institute of Astrophysics of the University of Liege has been present at the High Altitude Research Station Jungfraujoch, Switzerland, since the late 1940s, to perform spectrometric solar observations under dry and weakly polluted high-mountain conditions. Several solar atlases of photometric quality, extending altogether from the near-ultra-violet to the middle-infrared, were produced between 1956 and 1994, first with grating spectrometers then with Fourier transform instruments. During the early 1970s, scientific concerns emerged about atmospheric composition changes likely to set in as a consequence of the growing usage of nitrogen-containing agricultural fertilisers and the industrial production of chlorine-bearing compounds such as the chlorofluorocarbons and hydro-chlorofluorocarbons. Resulting releases to the atmosphere with ensuing photolysis in the stratosphere and catalytic depletion of the protective ozone layer prompted a worldwide consortium of chemical manufacturing companies to solicit the Liege group to help in clarifying these concerns by undertaking specific observations with its existing Jungfraujoch instrumentation. The following pages evoke the main steps that led from quasi full sun-oriented studies to priority investigations of the Earth's atmosphere, in support of both the Montreal and the Kyoto Protocols. [less ▲]

Evaluation of tropospheric and stratospheric ozone trends over Western Europe from ground-based FTIR network observations.

in Atmospheric Chemistry and Physics (2008), 362(8), 6865-6886

Ground-based CO observations at the Jungfraujoch: Comparison between FTIR and NDIR measurements

in Geophysical Research Abstracts (2008), 10

Measurements of CO have been performed at the Swiss Alpine Jungfraujoch station (46.5º N, 8.0° E, 3580m a.s.l.) on a regular basis since the mid-1980’s, using Fourier Transform Infrared solar absorption ... [more ▼]

Measurements of CO have been performed at the Swiss Alpine Jungfraujoch station (46.5º N, 8.0° E, 3580m a.s.l.) on a regular basis since the mid-1980’s, using Fourier Transform Infrared solar absorption spectrometry (FTIR), and since 1996 using an in situ Nondispersive Infrared technique (NDIR). While the in situ measurements detect local CO concentrations at the site, the FTIR technique provides integrated measurements along the line-of-sight. Nevertheless, the pressure broadening of the spectral absorption lines recorded at high resolution enables retrieving information on the vertical distribution of CO, mainly in the troposphere, including its concentration near the surface. Considering the inherent capabilities of the two independent measurement techniques, substantial differences between both data sets for surface level CO could potentially arise. Here we present a comparison of both data sets for the 1997 -2004 time period. Both data sets have been analysed by using successive Kolmogorov-Zurbenko filters. It appears that the long-term trend over the given time period is significantly different for both datasets. Possible causes for this difference will be critically discussed. [less ▲]

Impact of different spectroscopic datasets on CH4 retrievals from Jungfraujoch FTIR spectra

(2008)

Due to its high warming potential and its relatively long chemical lifetime (~9 years), atmospheric methane (CH4) plays a major role in the radiative forcing responsible of the greenhouse effect. Methane ... [more ▼]

Due to its high warming potential and its relatively long chemical lifetime (~9 years), atmospheric methane (CH4) plays a major role in the radiative forcing responsible of the greenhouse effect. Methane also affects climate by influencing tropospheric ozone and stratospheric water. High quality methane data sets are needed to understand its cycle and evaluate its budget of sources and sinks. Methane vertical distribution as well as total and partial column time series can be retrieved from high-resolution ground-based FTIR spectra, using, e.g., the SFIT-2 algorithm which implements the Optimal Estimation Method of Rodgers . However, although several retrieval approaches characterized by relatively high information content exist, methane retrieved profiles very often present large oscillations in their tropospheric range, which might result partly from inappropriate or inconsistent parameters. Significant improvements on retrieval quality should therefore be reached by using more accurate or compatible CH4 spectroscopic data. The main purpose of this contribution is to test and compare three different sets of CH4 spectroscopic parameters and to quantify their impact on CH4 retrieved products as well as on the fitting quality. [less ▲]

Retrievals of HCN from high-resolution FTIR solar spectra recorded at the Jungfraujoch station

in Geophysical Research Abstracts (2007, April)

Recent investigations have resulted in the revision of the lifetime of hydrogen cyanide (HCN) from 2.5 years to 2-5 months, more in line with its important and well documented variability in the ... [more ▼]

Recent investigations have resulted in the revision of the lifetime of hydrogen cyanide (HCN) from 2.5 years to 2-5 months, more in line with its important and well documented variability in the troposphere. The main HCN source is believed to be biomass burning, making this species a useful tracer of fires, e.g. the widespread and intense 2004 boreal fires. Oxidation by the OH radical is among the identified sinks, while uptake by oceans has been hypothesized as the dominant sink. As shown by previous investigations, several lines from the nu3 fundamental HCN band at 3 μm can be used to retrieve information on vertical distribution of hydrogen cyanide from high-resolution FTIR solar absorption spectra. The major interfering gas in this region is water vapor. A series of typical observations recorded at the Jungfraujoch station (46.5ºN, 8.0ºE, 3580m asl, Swiss Alps) by the NDACC (Network for the Detection of Atmospheric Composition Change)-affiliated Bruker instrument have been fitted using various approaches to determine the optimum strategy to be used for HCN retrievals at that site, even under very wet conditions. The selected approach is made of 7 windows encompassing 5 HCN lines. The a priori information (HCN vertical distribution and covariance matrix) is based on ACE-FTS measurements performed over northern midlatitudes. The HITRAN-2004 spectroscopic line parameters including the August 2006 updates for water vapor have been adopted in the retrievals performed with the OEM-SFIT-2 (v3.91) algorithm. This contribution will give a full description of the adopted retrieval approach, including error budget and information content analysis. Tropospheric column time series of HCN from 1994 onwards will also be presented and discussed. [less ▲]