Formic acid above the Jungfraujoch during 1985–2007: observed variability, seasonality, but no long-term background evolution
Zander, Rodolphe ; Duchatelet, Pierre ; Mahieu, Emmanuel et al
in Atmospheric Chemistry and Physics (2010), 10(20), 10047--10065
This paper reports on daytime total vertical column abundances of formic acid (HCOOH) above the Northern mid-latitude, high altitude Jungfraujoch station (Switzerland; 46.5° N, 8.0° E, 3580 m alt.). The ... [more ▼]
This paper reports on daytime total vertical column abundances of formic acid (HCOOH) above the Northern mid-latitude, high altitude Jungfraujoch station (Switzerland; 46.5° N, 8.0° E, 3580 m alt.). The columns were derived from the analysis of infrared solar observations regularly performed with high spectral resolution Fourier transform spectrometers during over 1500 days between September 1985 and September 2007. The investigation was based on the spectrometric fitting of five spectral intervals, one encompassing the HCOOH ν6 band Q branch at 1105 cm−1, and four additional ones allowing to optimally account for critical temperature-sensitive or time-evolving interferences by other atmospheric gases, in particular HDO, CCl2F2 and CHClF2. The main results derived from the 22 years long database indicate that the free tropospheric burden of HCOOH above the Jungfraujoch undergoes important short-term daytime variability, diurnal and seasonal modulations, inter-annual anomalies, but no significant long-term background change. A major progress in the remote determination of the atmospheric HCOOH columns reported here has resulted from the adoption of new, improved absolute spectral line intensities for the infrared ν6 band of trans-formic acid, resulting in retrieved free tropospheric loadings being about a factor two smaller than if derived with previous spectroscopic parameters. Implications of this significant change with regard to earlier remote measurements of atmospheric formic acid and comparison with relevant Northern mid-latitude findings, both in situ and remote, will be assessed critically. Sparse HCOOH model predictions will also be evoked and assessed with respect to findings reported here. [less ▲]Detailed reference viewed: 40 (12 ULg)
Optimized approach to retrieve information on the tropospheric and stratospheric carbonyl sulfide (OCS) vertical distributions above Jungfraujoch from high-resolution FTIR solar spectra
Lejeune, Bernard ; Mahieu, Emmanuel ; Servais, Christian et al
in Geophysical Research Abstracts (2010), 12(EGU2010-3513),
Carbonyl sulfide (OCS), which is produced in the troposphere from both biogenic and anthropogenic sources, is the most abundant gaseous sulfur species in the unpolluted atmosphere. Due to its low chemical ... [more ▼]
Carbonyl sulfide (OCS), which is produced in the troposphere from both biogenic and anthropogenic sources, is the most abundant gaseous sulfur species in the unpolluted atmosphere. Due to its low chemical reactivity and water solubility, a significant fraction of OCS is able to reach the stratosphere where it is converted to SO2 and ultimately to H2SO4 aerosols (Junge layer). These aerosols have the potential to amplify stratospheric ozone destruction on a global scale and may influence Earth’s radiation budget and climate through increasing solar scattering. The transport of OCS from troposphere to stratosphere is thought to be the primary mechanism by which the Junge layer is sustained during nonvolcanic periods. Because of this, long-term trends in atmospheric OCS concentration, not only in the troposphere but also in the stratosphere, are of great interest. A new approach has been developed and optimized to retrieve atmospheric abundance of OCS from high-resolution ground-based infrared solar spectra by using the SFIT-2 (v3.91) algorithm, including a new model for solar lines simulation (solar lines often produce significant interferences in the OCS microwindows). The strongest lines of the nu3 fundamental band of OCS at 2062 cm-1 have been systematically evaluated with objective criteria to select a new set of microwindows, assuming the HITRAN 2004 spectroscopic parameters with an increase in the OCS line intensities of the nu3band main isotopologue 16O12C32S by 15.79% as compared to HITRAN 2000 (Rothman et al., 2008, and references therein). Two regularization schemes have further been compared (deducted from ATMOS and ACE-FTS measurements or based on a Tikhonov approach), in order to select the one which optimizes the information content while minimizing the error budget. The selected approach has allowed us to determine updated OCS long-term trend from 1988 to 2009 in both the troposphere and the stratosphere, using spectra recorded on a regular basis with Fourier Transform Infrared spectrometers (FTIRs), under clear-sky conditions, at the NDACC site (Network for the Detection of Atmospheric Composition Change, visit http://www.ndacc.org) of the International Scientific Station of the Jungfraujoch (Swiss Alps, 46.5°N, 8.0°E, 3580m asl). Trends and seasonal cycles deduced from our results will be compared to values published in the literature and critically discussed. In particular, we will confirm the recent change in the OCS total column trend, which has become positive since 2002 before undergoing a slowing down over the last years. [less ▲]Detailed reference viewed: 97 (17 ULg)
An approach to retrieve information on the carbonyl fluoride (COF2) vertical distributions above Jungfraujoch by FTIR multi-spectrum multi-window fitting
Duchatelet, Pierre ; Mahieu, Emmanuel ; et al
in Atmospheric Chemistry and Physics (2009), 9
We present an original multi-spectrum fitting procedure to retrieve volume mixing ratio (VMR) profiles of carbonyl fluoride (COF2) from ground-based high resolution Fourier transform infrared (FTIR) solar ... [more ▼]
We present an original multi-spectrum fitting procedure to retrieve volume mixing ratio (VMR) profiles of carbonyl fluoride (COF2) from ground-based high resolution Fourier transform infrared (FTIR) solar spectra. The multi-spectrum approach consists of simultaneously combining, during the retrievals, all spectra recorded consecutively during the same day and with the same resolution. Solar observations analyzed in this study with the SFIT-2 v3.91 fitting algorithm correspond to more than 2900 spectra recorded between January 2000 and December 2007 at high zenith angles, with a Fourier Transform Spectrometer operated at the high-altitude International Scientific Station of the Jungfraujoch (ISSJ, 46.5° N latitude, 8.0° E longitude, 3580 m altitude), Switzerland. The goal of the retrieval strategy described here is to provide information about the vertical distribution of carbonyl fluoride. The microwindows used are located in the ν4 or in the ν4 COF2 infrared (IR) absorption bands. Averaging kernel and eigenvector analysis indicates that our FTIR retrieval is sensitive to COF2 inversion between 17 and 30 km, with the major contribution to the retrieved information always coming from the measurement. Moreover, there was no significant bias between COF2 partial columns, total columns or VMR profiles retrieved from the two bands. For each wavenumber region, a complete error budget including all identified sources has been carefully established. In addition, comparisons of FTIR COF2 17–30 km partial columns with KASIMA and SLIMCAT 3-D CTMs are also presented. If we do not notice any significant bias between FTIR and SLIMCAT time series, KASIMA COF2 17–30 km partial columns are lower of around 25%, probably due to incorrect lower boundary conditions. For each times series, linear trend estimation for the 2000–2007 time period as well as a seasonal variation study are also performed and critically discussed. For FTIR and KASIMA time series, very low COF2 growth rates (0.4±0.2%/year and 0.3±0.2%/year, respectively) have been derived. However, the SLIMCAT data set gives a slight negative trend (−0.5±0.2%/year), probably ascribable to discontinuities in the meteorological data used by this model. We further demonstrate that all time series are able to reproduce the COF2 seasonal cycle, which main seasonal characteristics deduced from each data set agree quite well. [less ▲]Detailed reference viewed: 85 (24 ULg)
Technical Note: Harmonized retrieval of column-integrated atmospheric water vapor from the FTIR network - First examples for long-term records and station trends
; ; et al
in Atmospheric Chemistry and Physics (2009), 9(22), 8987-8999
We present a method for harmonized retrieval of integrated water vapor (IWV) from existing, long-term, measurement records at the ground-based mid-infrared solar FTIR spectrometry stations of the Network ... [more ▼]
We present a method for harmonized retrieval of integrated water vapor (IWV) from existing, long-term, measurement records at the ground-based mid-infrared solar FTIR spectrometry stations of the Network for the Detection of Atmospheric Composition Change (NDACC). Correlation of IWV from FTIR with radiosondes shows an ideal slope of 1.00(3). This optimum matching is achieved via tuning one FTIR retrieval parameter, i.e., the strength of a Tikhonov regularization constraining the derivative (with respect to height) of retrieved water profiles given in per cent difference relative to an a priori profile. All other FTIR-sonde correlation parameters (intercept = 0.02(12) mm, bias = 0.02(5) mm, standard deviation of coincident IWV differences (stdv) = 0.27 mm, R = 0.99) are comparable to or better than results for all other ground-based IWV sounding techniques given in the literature. An FTIR-FTIR side-by-side intercomparison reveals a strong exponential increase in stdv as a function of increasing temporal mismatch starting at Δt ≈ 1 minute. This is due to atmospheric water vapor variability. Based on this result we derive an upper limit for the precision of the FTIR IWV retrieval for the smallest Δt (= 3.75 min) still giving a statistically sufficient sample (32 coincidences), i.e., precision (IWVFTIR) < 0.05 mm (or 2.2 % of the mean IWV). The bias of the IWV retrievals from the two different FTIR instruments is nearly negligible (0.02(1) mm). The optimized FTIR IWV retrieval is set up in the standard NDACC algorithm SFIT 2 without changes to the code. A concept for harmonized transfer of the retrieval between different stations deals with all relevant control parameters; it includes correction for differing spectral point spacings (via regularization strength), and final quality selection of the retrievals (excluding the highest residuals (measurement minus model), 5% of the total). As first application examples long-term IWV data sets are retrieved from the FTIR records of the Zugspitze (47.4 °N, 11.0 °E, 2964 m a.s.l.) and Jungfraujoch (46.5 °N, 8.0 °E, 3580 m a.s.l.) NDACC sites. Station-trend analysis comprises a linear fit after subtracting an intra-annual model (3 Fourier components) and constructing an uncertainty interval [95 % confidence] via bootstrap resampling. For the Zugspitze a significant trend of 0.79 [0.65, 0.92] mm/decade is found for the time interval [1996 - 2008], whereas for the Jungfraujoch no significant trend is found. This confirms recent findings that strong variations of IWV trends do occur above land on the local to regional scale (≈250 km) in spite of homogeneous surface temperature trends. This paper provides a basis for future exploitation of more than a dozen existing, multi-decadal FTIR measurement records around the globe for climate studies. [less ▲]Detailed reference viewed: 53 (13 ULg)
An FPGA-Based Data Acquisition and Processing System for the MATMOS FTIR Instrument.
; ; et al
in Proceedings - IEEE Aerospace Conference (2009), (1233), 11Detailed reference viewed: 24 (4 ULg)
Validation of ACE-FTS v2.2 measurements of HCl, HF, CCl3F and CCl2F2 using space-, balloon- and ground-based instrument observations
Mahieu, Emmanuel ; Duchatelet, Pierre ; Demoulin, Philippe et al
in Atmospheric Chemistry and Physics (2008), 8
Hydrogen chloride (HCl) and hydrogen fluoride (HF) are respectively the main chlorine and fluorine reservoirs in the Earth's stratosphere. Their buildup resulted from the intensive use of man-made ... [more ▼]
Hydrogen chloride (HCl) and hydrogen fluoride (HF) are respectively the main chlorine and fluorine reservoirs in the Earth's stratosphere. Their buildup resulted from the intensive use of man-made halogenated source gases, in particular CFC-11 (CCl3F) and CFC-12 (CCl2F2), during the second half of the 20th century. It is important to continue monitoring the evolution of these source gases and reservoirs, in support of the Montreal Protocol and also indirectly of the Kyoto Protocol. The Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) is a space-based instrument that has been performing regular solar occultation measurements of over 30 atmospheric gases since early 2004. In this validation paper, the HCl, HF, CFC-11 and CFC-12 version 2.2 profile data products retrieved from ACE-FTS measurements are evaluated. Volume mixing ratio profiles have been compared to observations made from space by MLS and HALOE, and from stratospheric balloons by SPIRALE, FIRS-2 and Mark-IV. Partial columns derived from the ACE-FTS data were also compared to column measurements from ground-based Fourier transform instruments operated at 12 sites. ACE-FTS data recorded from March 2004 to August 2007 have been used for the comparisons. These data are representative of a variety of atmospheric and chemical situations, with sounded air masses extending from the winter vortex to summer sub-tropical conditions. Typically, the ACE-FTS products are available in the 10-50 km altitude range for HCl and HF, and in the 7-20 and 7-25 km ranges for CFC-11 and -12, respectively. For both reservoirs, comparison results indicate an agreement generally better than 5-10% above 20 km altitude, when accounting for the known offset affecting HALOE measurements of HCl and HF. Larger positive differences are however found for comparisons with single profiles from FIRS-2 and SPIRALE. For CFCs, the few coincident measurements available suggest that the differences probably remain within +/-20%. [less ▲]Detailed reference viewed: 89 (32 ULg)
Our Changing Atmosphere: Evidence Based on Long-Term Infrared Solar Observations at the Jungfraujoch since 1950
Zander, Rodolphe ; Mahieu, Emmanuel ; Demoulin, Philippe et al
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 ▲]Detailed reference viewed: 58 (29 ULg)
H2O retrievals from Jungfraujoch infrared spectra: some spectroscopic problems.
Demoulin, Philippe ; ; Mahieu, Emmanuel et al
in Proceedings of the 8th Atmospheric Spectroscopy Applications Meeting (2008)
Since 1949, solar absorption spectra have been acquired at the Jungfraujoch observatory (Swiss Alps, 46.5°N, 8.0°E, 3580 m a.s.l.), first with grating spectrometers, then with Fourier transform infrared ... [more ▼]
Since 1949, solar absorption spectra have been acquired at the Jungfraujoch observatory (Swiss Alps, 46.5°N, 8.0°E, 3580 m a.s.l.), first with grating spectrometers, then with Fourier transform infrared (FTIR) spectrometers. Most observations collected with these instruments encompass water vapor absorptions, even the narrow spectral domains regularly recorded with the grating instruments to monitor the evolution of important atmospheric constituents. The aim of this work is to analyze all available spectra containing usable H2O absorption lines, to derive a long-term record of its total column in the atmosphere above the Jungfraujoch. In addition, more recent FTIR broadband spectra, with better signal-to-noise ratio and resolution, will be analyzed with state of the art algorithm, in order to derive information on the vertical distribution of H2O. [less ▲]Detailed reference viewed: 28 (4 ULg)
Evaluation of tropospheric and stratospheric ozone trends over Western Europe from ground-based FTIR network observations.
; ; Demoulin, Philippe et al
in Atmospheric Chemistry and Physics (2008), 362(8), 6865-6886Detailed reference viewed: 55 (4 ULg)
Optimized approaches to invert Jungfraujoch high-resolution FTIR observations for long-term monitoring and satellite validation of tropospheric species.
Mahieu, Emmanuel ; Servais, Christian ; Duchatelet, Pierre et al
Report (2008)Detailed reference viewed: 12 (2 ULg)
Retrievals of C2H2 from high-resolution FTIR solar spectra recorded at the Jungfraujoch station (46.5ºN) and comparison with ACE-FTS observations
Mahieu, Emmanuel ; Duchatelet, Pierre ; et al
in Geophysical Research Abstracts (2008), 10
Acetylene (C2H2) is among the nonmethane hydrocarbons (NMHCs) accessible to infrared remote sensing technique. As a product of combustion and biomass burning, it is emitted at the Earth’s surface and ... [more ▼]
Acetylene (C2H2) is among the nonmethane hydrocarbons (NMHCs) accessible to infrared remote sensing technique. As a product of combustion and biomass burning, it is emitted at the Earth’s surface and further transported and mixed into the troposphere. Destruction by OH is the main removal process. The average tropospheric lifetime of C2H2 is estimated at about 1 month on the global scale; at mid-latitudes, it varies between 20 days in summer to 160 days in winter. This compound is appropriate to study tropospheric pollution and transport, and is often used in conjunction with other tracers of fires. C2H2 presents exploitable infrared absorption features near 3 and 15 μm, where weak isolated lines of the nu5 and the nu2 + nu4 + nu5 bands are found, respectively. Several of these lines can be used to retrieve abundances of C2H2 from high-resolution groundbased infrared solar spectra. 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 with the OEM-SFIT-2 (v3.91) algorithm. Various approaches and combination of lines have been tested, seeking for the optimum inversion strategy. The HITRAN-2004 spectroscopic line parameters including the August 2006 updates for water vapor have been adopted in the retrievals. These approaches will be presented and critically compared, with the help of error budget and information content analyses, taking into account the impact of major interferences such as water vapor. The time series of C2H2 tropospheric column abundances above Jungfraujoch will also be presented, including determination of its long-term trend and strong seasonal cycle. The ground-based results will further be compared with zonal mean observations performed by the ACE-FTS space-based instrument since early 2004. [less ▲]Detailed reference viewed: 74 (6 ULg)
Retrievals of HCN from high-resolution FTIR solar spectra recorded at the Jungfraujoch station
Mahieu, Emmanuel ; Duchatelet, Pierre ; Demoulin, Philippe et al
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 ▲]Detailed reference viewed: 78 (7 ULg)
FTIR Observations at the Jungfraujoch Station for long-term monitoring of the Troposphere and Validation of the Space-based Sensors.
Mahieu, Emmanuel ; Zander, Rodolphe ; Demoulin, Philippe et al
in Burrows, J.; Borrell, P. (Eds.) Measuring Tropospheric Trace Constituents from Space. (2007)Detailed reference viewed: 20 (8 ULg)
Optimisation of retrieval strategies using Jungfraujoch high-resolution FTIR observations for long-term trend studies and satellite validation.
Mahieu, Emmanuel ; Servais, Christian ; Duchatelet, Pierre et al
in Burrows, J.; Borrell, P. (Eds.) Observing Tropospheric Trace Constituents from Space. (2007)Detailed reference viewed: 7 (2 ULg)
A remotely actuated suntracker protection for harsh environmental conditions.
Servais, Christian ; Demoulin, Philippe ; Flock, Olivier et al
(2007)Detailed reference viewed: 9 (4 ULg)
FTIR signal acquisition based on simultaneous analog sampling of the laser reference and IR detectors.
Servais, Christian ; ; et al
Scientific conference (2007)Detailed reference viewed: 23 (9 ULg)
IR signal DC coupling and Source Intensity variation compensation from the hardware point of view.
Scientific conference (2007)Detailed reference viewed: 9 (1 ULg)
A new software framework specially designed for remote FTIR observation.
Servais, Christian ; Flock, Olivier ; Demoulin, Philippe
Scientific conference (2007)Detailed reference viewed: 10 (3 ULg)
AURA validation by the baloon-borne MkIV Interferometer.
; ; et al
Scientific conference (2006)Detailed reference viewed: 7 (1 ULg)
Evolution of a dozen non-CO2 greenhouse gases above Central Europe since the mid-1980s.
Zander, Rodolphe ; Mahieu, Emmanuel ; Demoulin, Philippe et al
in Proceedings of the 4th International Symposium on Non-CO2 Greenhouse Gases (2006)Detailed reference viewed: 13 (3 ULg)