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See detailLong-term trends of a dozen direct greenhouse gases derived from infrared solar absorption spectra recorded at the Jungfraujoch station
Mahieu, Emmanuel ULg; Duchatelet, Pierre; Zander, Rodolphe ULg et al

Poster (2011, November 10)

References Bader, W. et al., Extension of the long-term total column time series of atmospheric methane above the Jungfraujoch station: analysis of grating infrared spectra between 1976 and 1989 ... [more ▼]

References Bader, W. et al., Extension of the long-term total column time series of atmospheric methane above the Jungfraujoch station: analysis of grating infrared spectra between 1976 and 1989, Geophysical Research Abstracts, 13, EGU2011-3391-1, 2011. [http://hdl.handle.net/2268/88180] Duchatelet, P. et al., First retrievals of carbon tetrafluoride (CF4) from ground-based FTIR measurements: production and analysis of the two-decadal time series above the Jungfraujoch, Geophysical Research Abstracts, 13, EGU2011-6413, 2011. [http://hdl.handle.net/2268/90745] Gardiner, T. et al., Trend analysis of greenhouse gases over Europe measured by a network of ground-based remote FTIR instruments, Atmos. Chem. Phys., 8, 6719-6727, 2008. [http://hdl.handle.net/2268/2545] Rodgers, C.D., Characterisation and error analysis of profiles derived from remote sensing measurements, J. Geophys. Res., 95, 5587-5595, 1990. Zander, R. et al., Our changing atmosphere: Evidence based on long-term infrared solar observations at the Jungfraujoch since 1950, Sci. Total Environ., 391, 184-195, 2008. [http://hdl.handle.net/2268/2421] [less ▲]

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See detailFirst retrievals of methyl chloride from ground-based high-resolution FTIR solar observations
Mahieu, Emmanuel ULg; Harrison, Jeremy; Bernath, Peter F. et al

in Geophysical Research Abstracts (2011), 13

Methyl chloride (CH3Cl) is one of the most abundant chlorine-bearing gas in the Earth’s troposphere and a significant contributor to the organic chlorine budget. Measurements by in situ networks indicate ... [more ▼]

Methyl chloride (CH3Cl) is one of the most abundant chlorine-bearing gas in the Earth’s troposphere and a significant contributor to the organic chlorine budget. Measurements by in situ networks indicate a mean volume mixing ratio of 550 pptv, with a significant seasonal cycle of about 80 pptv, peak to peak. This species also exhibits inter-annual variability, but no long-term trend. Major sources are from tropical and sub-tropical plants and dead leaves, the oceans and biomass burning. Some industrial processes and waste incineration further add to the emissions. Oxidation by the hydroxyl radical is by far the largest CH3Cl sink, followed by soil uptake. Although balanced, its atmospheric budget is still affected by large uncertainties and contributions from unidentified sources and sinks cannot be ruled out. Methyl chloride has an atmospheric lifetime of 1 year, a global warming potential of 13 (100-yr horizon) and an ozone depleting potential of 0.02. The retrieval of methyl chloride from ground-based infrared (IR) spectra is very challenging. Indeed, numerous interferences by strong water vapor and methane lines complicate the detection of small CH3Cl absorptions, close to 1%, near 3 microns. In addition, and although weak, ethane features contribute to the difficulty, in particular since a significant number of ethane branches were absent until very recently from official HITRAN compilations. Therefore, the scientific literature does not report thus far about any investigations of CH3Cl from ground-based remote sensing observations. In this contribution, we will present first CH3Cl total column retrievals, using the SFIT-2 algorithm (v3.94) and high-resolution Fourier Transform Infrared (FTIR) solar absorption observations recorded with a Bruker 120HR instrument, at the high altitude station of the Jungfraujoch (46.5°N, 8°E, 3580 m asl), within the framework of the Network for the Detection of Atmospheric Composition Change (NDACC, visit http://www.ndacc.org). In our retrievals, we use new ethane absorption cross sections recorded at the Molecular Spectroscopy Facility of the Rutherford Appleton Laboratory (Harrison et al., 2010). They were calibrated in intensity by using reference low-resolution spectra from the Pacific Northwest National Laboratory (PNNL) IR database. These new cross sections were recently released as a HITRAN update (see http://www.hitran.com). Pseudoline parameters fitted to these ethane spectra have been combined with HITRAN 2004 line parameters (including all the 2006 updates) for all other species encompassed in the selected microwindows, including our target CH3Cl. We will evaluate the improvement brought by the new ethane line parameters on the fitting residuals, and characterize the quality, the precision and the reliability of the retrieved product. If successful, a long-term CH3Cl total column time series will be produced using the Jungfraujoch observational database, and we will perform preliminary investigations of the seasonal and inter-annual variations of methyl chloride total columns at northern mid-latitudes. [less ▲]

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See detailLong-term trend of carbon tetrachloride (CCl4) from ground-based high resolution infrared solar spectra recorded at the Jungfraujoch
Rinsland, Curtis P.; Mahieu, Emmanuel ULg; Demoulin, Philippe ULg et al

in Geophysical Research Abstracts (2010), 12(EGU2010-1819-3),

The long-term trend of carbon tetrachloride (CCl4) has been retrieved from infrared high resolution solar absorption spectra encompassing the 1999 to 2010 time period. The measurements were recorded with ... [more ▼]

The long-term trend of carbon tetrachloride (CCl4) has been retrieved from infrared high resolution solar absorption spectra encompassing the 1999 to 2010 time period. The measurements were recorded with a Fourier transform spectrometer at the northern mid-latitude, high altitude Jungfraujoch station in Switzerland (46.5°N latitude, 8.0°E longitude, 3580 m altitude). Total columns were derived from the region of the strong CCl4 _3 band at 794 cm􀀀1 accounting for all interfering molecules (e.g. H2O, O3) with significant improvement in the residuals obtained by also taking into account the line mixing in a nearby CO2 Q branch, a procedure not implemented in previous remote sensing CCl4 retrievals though its importance has been noted in several papers. The time series shows a statistically-significant long-term decrease in the CCl4 total atmospheric burden of -1.18_0.10 %/yr, at the 95% confidence level, using 2005 as reference. Furthermore, fit to the total column data set also reveals a seasonal cycle with a peak-to-peak amplitude of 10.2%, with minimum and maximum values found in mid-February and early August, respectively. This seasonal modulation can however be attributed to tropopause height changes throughout the season. The results quantify the continued impact of the regulations implemented by the Montreal Protocol and its strengthening amendments and adjustments for a molecule with high global warming potential. Although a statistically significant decrease in the total column is inferred, the CCl4 molecule remains an important contributor to the stratospheric chlorine budget and burden. [less ▲]

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See detailRecent trends of inorganic chlorine and halogenated source gases above the Jungfraujoch and Kitt Peak stations derived from high-resolution FTIR solar observations
Mahieu, Emmanuel ULg; Rinsland, Curtis P.; Gardiner, Tom et al

in Geophysical Research Abstracts (2010), 12(EGU2010-2420-3),

The longest series of Fourier Transform Infrared (FTIR) high spectral resolution solar absorption observations are available from the Jungfraujoch and Kitt Peak stations, located at 46.5ºN and 30.9ºN ... [more ▼]

The longest series of Fourier Transform Infrared (FTIR) high spectral resolution solar absorption observations are available from the Jungfraujoch and Kitt Peak stations, located at 46.5ºN and 30.9ºN, respectively. State-of-the-art interferometers are operated at these sites within the framework of the Network for the Detection of Atmospheric Composition Change (NDACC, visit http://www.ndacc.org). These instruments allow to record spectra on a regular basis, under clear-sky conditions, using a suite of optical filters which altogether cover the 2 to 16 micron spectral range. Numerous absorption features characterized in the HITRAN compilations (e.g. Rothman et al., 2008) are encompassed in this mid-infrared region. Their analyses with either the SFIT-1 or SFIT-2 algorithm allow retrieving total columns of the target gases. Moreover, information on their distribution with altitude can generally be derived when using SFIT-2 which implements the Optimal Estimation Method of Rodgers (1990). Among the two dozen gases of atmospheric interest accessible to the ground-based FTIR technique, we have selected here a suite of long-lived halogenated species: HCl, ClONO2, CCl2F2, CCl3F, CHClF2, CCl4 and SF6. Time series available from the two sites will be presented, compared and critically discussed. In particular, changes in the abundances of theses gases since the peak in inorganic chlorine (Cly, which occurred in 1996-1997) and their intra-annual variability will be characterized with a statistical tool using bootstrap resampling (Gardiner et al., 2008). Trends and their associated uncertainties will be reported and put into perspective with the phase-out regulations of the production of ozone depleting substances adopted and implemented by the Montreal Protocol, its Amendments and Adjustments. For instance, the trends affecting the reservoir species HCl, ClONO2, and their summation which is a good proxy of the total inorganic chlorine, have been calculated using all available daily mean measurements from January 1996 onwards. The following values were obtained for Jungfraujoch, when using 1996 as the reference year: -0.90±0.10%/yr for HCl, -0.92±0.26 %/yr for ClONO2, and -0.96±0.14 %/yr for Cly; in all cases, the uncertainties define the 95% confidence interval around the trend values. For Kitt Peak, the corresponding trends are: -0.55±0.34 %/yr for HCl, -1.27±0.84 %/yr for ClONO2 and -0.61±0.51 %/yr for Cly, they are statistically consistent with the Jungfraujoch rates of decrease. Further trend data will be presented at the EGU General Assembly while supplementary information on Jungfraujoch results will be available from communications at the same meeting by Duchatelet et al. (2010), Lejeune et al (2010) and Rinsland et al (2010). Comparisons with model data are also foreseen. [less ▲]

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See detailTrend of lower stratospheric methane (CH4) from Atmospheric Chemistry Experiment (ACE) and Atmospheric Trace Molecule Spectroscopy (ATMOS) measurements
Rinsland, Curtis P.; Chiou, Linda S.; Boone, C. D. et al

in Journal of Quantitative Spectroscopy & Radiative Transfer (2009), 110(13), 1066-1071

The long-term trend of methane (CH4) in the lower stratosphere has been estimated for the 1985 to 2008 time period by combining spaceborne solar occultation measurements recorded with high spectral ... [more ▼]

The long-term trend of methane (CH4) in the lower stratosphere has been estimated for the 1985 to 2008 time period by combining spaceborne solar occultation measurements recorded with high spectral resolution Fourier transform spectrometers (FTSs). Volume mixing ratio (VMR) FTS measurements from the ATMOS (Atmospheric Trace Molecule Spectroscopy) FTS covering 120-10 hPa (~16 to 30 km altitude) at 25°N-35°N latitude from 1985 and 1994 have been combined with Atmospheric Chemistry Experiment (ACE) SCISAT-1 FTS measurements covering the same latitude and pressure range from 2004 to 2008. The CH4 trend was estimated by referencing the VMRs to those measured for the long-lived constituent N2O to account for the dynamic history of the sampled airmasses. The combined measurement set shows that the VMR increase measured by ATMOS has been replaced by a leveling off during the ACE measurement time period. Our conclusion is consistent with both remote sensing and in situ measurements of the CH4 trend obtained over the same time span. [less ▲]

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See detailFirst ground-based infrared solar absorption measurements of free tropospheric methanol (CH3OH): Multidecade infrared time series from Kitt Peak (31.9°N 111.6°W), trend, seasonal cycle, and comparison with previous measurements
Rinsland, Curtis P.; Mahieu, Emmanuel ULg; Chiou, Linda et al

in Journal of Geophysical Research (2009), 114(D04309),

Atmospheric CH3OH (methanol) free tropospheric (2.09-14 km altitude) time series spanning 22 years has been analyzed based on high spectral resolution infrared solar absorption spectra of the strong ν8 ... [more ▼]

Atmospheric CH3OH (methanol) free tropospheric (2.09-14 km altitude) time series spanning 22 years has been analyzed based on high spectral resolution infrared solar absorption spectra of the strong ν8 band recorded from the U.S. National Solar Observatory on Kitt Peak (latitude 31.9°N, 111.6°W, 2.09 km altitude) with a 1-m Fourier transform spectrometer (FTS). The measurements span October 1981 to December 2003 and are the first long time series of CH3OH measurements obtained from the ground. The results were analyzed with SFIT2 version 3.93 and show a factor of three variations with season, a maximum at the beginning of July, a winter minimum, and no statistically significant long-term trend over the measurement time span. [less ▲]

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See detailFirst measurements of the HCFC-142b trend from atmospheric chemistry experiment (ACE) solar occultation spectra
Rinsland, Curtis P; Chiou, Linda; Boone, Chris et al

in Journal of Quantitative Spectroscopy & Radiative Transfer (2009), 110(18), 2127-2134

The first measurement of the HCFC-142b (CH3CClF2) trend near the tropopause has been derived from volume mixing ratio (VMR) measurements at northern and southern hemisphere mid-latitudes for the 2004-2008 ... [more ▼]

The first measurement of the HCFC-142b (CH3CClF2) trend near the tropopause has been derived from volume mixing ratio (VMR) measurements at northern and southern hemisphere mid-latitudes for the 2004-2008 time period from spaceborne solar occultation observations recorded at 0.02 cm(-1) resolution with the ACE (atmospheric chemistry experiment) Fourier transform spectrometer. The HCFC-142b molecule is currently the third most abundant HCFC (hydrochlorofluorocarbon) in the atmosphere and ACE measurements over this time span show a continuous rise in its volume mixing ratio. Monthly average measurements at northern and southern hemisphere mid-latitudes have similar increase rates that are consistent with surface trend measurements for a similar time span. A mean northern hemisphere profile for the time span shows a near constant VMR at 8-20 km altitude range, consistent on average for the same time span with in situ results. The nearly constant vertical VMR profile also agrees with model predictions of a long lifetime in the lower atmosphere. (c) 2009 Elsevier Ltd. All rights reserved. [less ▲]

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See detailMeasurements of long-term changes in atmospheric OCS (carbonyl sulfide) from infrared solar observations
Rinsland, Curtis P.; Chiou, Linda S.; Mahieu, Emmanuel ULg et al

in Journal of Quantitative Spectroscopy & Radiative Transfer (2008), 109(16), 2679-2686

Multi-decade atmospheric OCS (carbonyl sulfide) infrared measurements have been analyzed with the goal of quantifying long-term changes and evaluating the consistency of the infrared atmospheric OCS ... [more ▼]

Multi-decade atmospheric OCS (carbonyl sulfide) infrared measurements have been analyzed with the goal of quantifying long-term changes and evaluating the consistency of the infrared atmospheric OCS remote-sensing measurement record. Solar-viewing grating spectrometer measurements recorded in April 1951 at the Jungfraujoch station (46.5°N latitude, 8.0°E longitude, 3.58 km altitude) show evidence for absorption by lines of the strong ν3 band of OCS at 2062 cm(−1). The observation predates the earliest previously reported OCS atmosphere remote-sensing measurement by two decades. More recent infrared ground-based measurements of OCS have been obtained primarily with high-resolution solar-viewing Fourier transform spectrometers (FTSs). Long-term trends derived from this record span more than two decades and show OCS columns that have remained constant or have decreased slightly with time since the Mt. Pinatubo eruption, though retrievals assuming different versions of public spectroscopic databases have been impacted by OCS ν3 band line intensity differences of 10%. The lower stratospheric OCS trend has been inferred assuming spectroscopic parameters from the high-resolution transmission (HITRAN) 2004 database. Volume mixing ratio (VMR) profiles measured near 30°N latitude with high-resolution solar-viewing FTSs operating in the solar occultation mode over a 22 years time span were combined. Atmospheric Trace MOlecucle Spectroscopy (ATMOS) version 3 FTS measurements in 1985 and 1994 were used with Atmospheric Chemistry Experiment (ACE) measurements during 2004–2007. Trends were calculated by referencing the measured OCS VMRs to those of the long-lived constituent N2O to account for variations in the dynamic history of the sampled airmasses. Means and 1-sigma standard deviations of VMRs (in ppbv, or 10−9 per unit air volume) averaged over 30–100 hPa from measurements at 25–35°N latitude are 0.334±0.089 ppbv from 1985 (ATMOS Spacelab 3 measurements), 0.297±0.094 ppbv from 1994 ATLAS 3 measurements, 0.326±0.074 ppbv from ACE 2004 measurements, 0.305±0.096 ppbv from ACE 2005 measurements, 0.328±0.074 from ACE 2006 measurements, and 0.305±0.090 ppbv from ACE measurements through August 2007. Assuming these parameters, we conclude that there has been no statistically significant trend in lower stratospheric OCS over the measurement time span. We discuss past measurement sets, quantify the impact of changes in infrared spectroscopic parameters on atmospheric retrievals and trend measurements, and discuss OCS spectroscopic uncertainties of the current ν3 band parameters in public atmospheric databases. [less ▲]

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See detailValidation of ACE-FTS v2.2 measurements of HCl, HF, CCl3F and CCl2F2 using space-, balloon- and ground-based instrument observations
Mahieu, Emmanuel ULg; Duchatelet, Pierre ULg; Demoulin, Philippe ULg 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 ▲]

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See detailCO measurements from the ACE-FTS satellite instrument: data analysis and validation using ground-based, airborne and spaceborne observations
Clerbaux, Catherine; George, Maya; Turquety, Solène et al

in Atmospheric Chemistry and Physics (2008), 8

The Atmospheric Chemistry Experiment (ACE) mission was launched in August 2003 to sound the atmosphere by solar occultation. Carbon monoxide (CO), a good tracer of pollution plumes and atmospheric ... [more ▼]

The Atmospheric Chemistry Experiment (ACE) mission was launched in August 2003 to sound the atmosphere by solar occultation. Carbon monoxide (CO), a good tracer of pollution plumes and atmospheric dynamics, is one of the key species provided by the primary instrument, the ACE-Fourier Transform Spectrometer (ACE-FTS). This instrument performs measurements in both the CO 1-0 and 2-0 ro-vibrational bands, from which vertically resolved CO concentration profiles are retrieved, from the mid-troposphere to the thermosphere. This paper presents an updated description of the ACE-FTS version 2.2 CO data product, along with a comprehensive validation of these profiles using available observations (February 2004 to December 2006). We have compared the CO partial columns with ground-based measurements using Fourier transform infrared spectroscopy and millimeter wave radiometry, and the volume mixing ratio profiles with airborne (both high-altitude balloon flight and airplane) observations. CO satellite observations provided by nadir-looking instruments (MOPITT and TES) as well as limb-viewing remote sensors (MIPAS, SMR and MLS) were also compared with the ACE-FTS CO products. We show that the ACE-FTS measurements provide CO profiles with small retrieval errors (better than 5% from the upper troposphere to 40 km, and better than 10% above). These observations agree well with the correlative measurements, considering the rather loose coincidence criteria in some cases. Based on the validation exercise we assess the following uncertainties to the ACE-FTS measurement data: better than 15% in the upper troposphere (8–12 km), than 30% in the lower stratosphere (12–30 km), and than 25% from 30 to 100 km. [less ▲]

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See detailOur Changing Atmosphere: Evidence Based on Long-Term Infrared Solar Observations at the Jungfraujoch since 1950
Zander, Rodolphe ULg; Mahieu, Emmanuel ULg; Demoulin, Philippe ULg 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 ▲]

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See detailSpectroscopic detection of COClF in the tropical and mid-latitude lower stratosphere
Rinsland, Curtis P.; Nassar, Ray; Boone, Christopher D. et al

in Journal of Quantitative Spectroscopy & Radiative Transfer (2007), 105(3), 467-475

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 ... [more ▼]

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(-12) per unit volume, 1 sigma) is measured at 28 km for tropical and subtropical occultations (latitudes below 20 degrees in both hemispheres) with lower mixing ratios at both higher and lower altitudes. Northern hemisphere mid-latitude mixing ratios (30-50 degrees N) resulted in an average profile with a peak mixing ratio of 51.7 +/- 132.1 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 (2.5-4.5 km offset) than in the model prediction. Seasonal average 2-D-model predictions of the COClF stratospheric distribution for 2004 are also reported. (c) 2006 Elsevier Ltd. All rights reserved. [less ▲]

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See detailLong-term trends of tropospheric carbon monoxide and hydrogen cyanide from analysis of high resolution infrared solar spectra
Rinsland, Curtis P.; Goldman, Aaron; Hannigan, James W. et al

in Journal of Quantitative Spectroscopy & Radiative Transfer (2007), 104(1), 40-51

Long-term trend and seasonal variation of the mean free tropospheric volume mixing ratios of carbon monoxide (CO) and hydrogen cyanide (HCN) have been derived from analysis of a time series of solar ... [more ▼]

Long-term trend and seasonal variation of the mean free tropospheric volume mixing ratios of carbon monoxide (CO) and hydrogen cyanide (HCN) have been derived from analysis of a time series of solar absorption spectra recorded from the US National Solar Observatory on Kitt Peak (31.9 degrees N, 111.6 degrees W, 2.09 km altitude) spanning almost three decades. The results of a fit to the CO 258 daily averages from May 1977 to April 2005 as a function of time with a model that assumes a sinusoidal seasonal cycle and a linear long-term trend with time yield a mean volume mixing ratio of 102 +/- 3) parts per billion (10(-9) per unit volume) below 10km altitude, I sigma. The CO measurements show a seasonal cycle with a maximum in March and a minimum in September with an amplitude of (22.3 +/- 1.5)% relative to the mean. The best-fit corresponds to a long-term CO trend of (0.15 +/- 0.14)% yr(-1), 1 sigma, relative to the mean. To quantify the possible impact of periods of intense fires, the CO measurements have been compared with the measurements of HCN, a well-documented emission product of biomass burning with a lifetime of similar to 5 months. The best fit to the full HCN time series of 208 daily averages from May 1978 to April 2005 results in a mean volume mixing ratio of (0.219 +/- 0.007) ppbv below 10 km altitude with a similar seasonal cycle, though with a lower relative amplitude than for CO. Although same-day enhancements up to a factor of 1.87 for HCN and 1.24 for CO were measured relative to values predicted by a fit to the time series that accounts for the seasonal cycles and trends of both molecules, excluding time periods of elevated fire emissions has no significant impact on the best-fit long-term free tropospheric CO and HCN trends. Our result of no long-term CO trend since the late 1970s suggests that the global average long-term decline reported from 1990 through 1995 measurements has not continued in the free troposphere. Similarly, a fit to the full time series of 208 HCN free tropospheric daily averages with the same model yields an average 2.09-10km mixing ratio of 0.219ppbv and a long-term trend of (-0.12 +/- 0.14) % yr(-1), 1 sigma, relative to the mean since 1978, also indicating no significant long-term trend above the lower mid-latitude continental US Kitt Peak station. The results for both molecules suggest the site was not significantly impacted by summer boreal fires during the time span of the measurements that in some years cause widespread pollution above northern higher latitude sites. (c) 2006 Elsevier Ltd. All rights reserved. [less ▲]

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See detailFirst space-based observations of formic acid (HCOOH): Atmospheric Chemistry Experiment austral spring 2004 and 2005 Southern Hemisphere tropical-mid-latitude upper tropospheric measurements
Rinsland, Curtis P.; Boone, Christopher D.; Bernath, Peter F. et al

in Geophysical Research Letters (2006), 33(23),

The first space-based measurements of upper tropospheric ( 110 - 300 hPa) formic acid (HCOOH) are reported from 0.02 cm(-1) resolution Atmospheric Chemistry Experiment (ACE) Fourier transform spectrometer ... [more ▼]

The first space-based measurements of upper tropospheric ( 110 - 300 hPa) formic acid (HCOOH) are reported from 0.02 cm(-1) resolution Atmospheric Chemistry Experiment (ACE) Fourier transform spectrometer solar occultation measurements at 16 degrees S - 43 degrees S latitude during late September to early October in 2004 and 2005. A maximum upper tropospheric HCOOH mixing ratio of 3.13 +/- 0.02 ppbv ( 1 ppbv = 10(-9) per unit volume), 1 sigma, at 10.5 km altitude was measured during 2004 at 29.97 degrees S latitude and a lower maximum HCOOH mixing ratio of 2.03 +/- 0.28 ppbv, at 9.5 km altitude was measured during 2005. Fire counts, back trajectories, and correlations of HCOOH mixing ratios with ACE simultaneous measurements of other fire products confirm the elevated HCOOH mixing ratios originated primarily from tropical fire emissions. A HCOOH emission factor relative to CO of 1.99 +/- 1.34 g kg(-1) during 2004 in upper tropospheric plumes is inferred from a comparison with lower mixing ratios measured during the same time period assuming HITRAN 2004 spectroscopic parameters. [less ▲]

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See detailA global inventory of stratospheric fluorine in 2004 based on Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) measurements
Nassar, Ray; Bernath, Peter F.; Boone, Christopher D. et al

in Journal of Geophysical Research (2006), 111

Total fluorine (FTOT) in the stratosphere has been determined using Atmospheric Chemistry Experiment Fourier transform spectrometer (ACE-FTS) measurements of HF, COF2, COClF, CF4, CCl3F (CFC-11), CCl2F2 ... [more ▼]

Total fluorine (FTOT) in the stratosphere has been determined using Atmospheric Chemistry Experiment Fourier transform spectrometer (ACE-FTS) measurements of HF, COF2, COClF, CF4, CCl3F (CFC-11), CCl2F2 (CFC-12), CHClF2 (HCFC-22), CCl2FCClF2 (CFC-113), CH3CClF2 (HCFC-142b), CH2FCF3 (HFC-134a), and SF6. The retrieval of HFC-134a (CH2FCF3) from spaceborne measurements had not been carried out prior to this work. Measurements of these species have been supplemented by data from models to extend the altitude range of the profiles and have also been complemented by estimates of 15 minor fluorine species. Using these data, separate fluorine budgets were determined in five latitude zones (60°–82°N, 30°–60°N, 30°S–30°N, 30°–60°S, and 60°–82°S) by averaging over the period of February 2004 to January 2005 inclusive, when possible. Stratospheric FTOT profiles in each latitude zone are nearly linear, with mean stratospheric FTOT values ranging from 2.50 to 2.59 ppbv (with a 1sig precision of 0.04–0.07 ppbv and an estimated accuracy of 0.15 ppbv) for each zone. The highest mean FTOT value occurred in the tropics, which is qualitatively consistent with increasing levels of stratospheric fluorine and the mean stratospheric circulation pattern. [less ▲]

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See detailA global inventory of stratospheric chlorine in 2004
Nassar, Ray; Bernath, Peter; Boone, Christopher D. et al

in Journal of Geophysical Research. Atmospheres (2006), 111(D22), 22312

[1] Total chlorine (Cl-TOT) in the stratosphere has been determined using the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) measurements of HCl, ClONO2, CH3Cl, CCl4, CCl3F (CFC ... [more ▼]

[1] Total chlorine (Cl-TOT) in the stratosphere has been determined using the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) measurements of HCl, ClONO2, CH3Cl, CCl4, CCl3F (CFC-11), CCl2F2 (CFC-12), CHClF2 (HCFC-22), CCl2FCClF2 (CFC-113), CH3CClF2 (HCFC-142b), COClF, and ClO supplemented by data from several other sources, including both measurements and models. Separate chlorine inventories were carried out in five latitude zones (60 degrees - 82 degrees N, 30 degrees - 60 degrees N, 30 degrees S - 30 degrees N, 30 degrees - 60 degrees S, and 60 degrees - 82 degrees S), averaging the period of February 2004 to January 2005 inclusive, when possible, to deal with seasonal variations. The effect of diurnal variation was avoided by only using measurements taken at local sunset. Mean stratospheric Cl-TOT values of 3.65 ppbv were determined for both the northern and southern midlatitudes (with an estimated 1 sigma accuracy of +/- 0.13 ppbv and a precision of +/- 0.09 ppbv), accompanied by a slightly lower value in the tropics and slightly higher values at high latitudes. Stratospheric Cl-TOT profiles in all five latitude zones are nearly linear with a slight positive slope in ppbv/km. Both the observed slopes and pattern of latitudinal variation can be interpreted as evidence of the beginning of a decline in global stratospheric chlorine, which is qualitatively consistent with the mean stratospheric circulation pattern and time lag necessary for transport. [less ▲]

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See detailComparisons between SCIAMACHY and ground-based FTIR data for total columns of CO, CH4, CO2 and N2O
Dils, Bart; De Mazière, Martine; Muller, Jean-François et al

in Atmospheric Chemistry and Physics (2006), 6

Total column amounts of CO, CH4, CO2 and N2O retrieved from SCIAMACHY nadir observations in its near-infrared channels have been compared to data from a ground-based quasi-global network of Fourier ... [more ▼]

Total column amounts of CO, CH4, CO2 and N2O retrieved from SCIAMACHY nadir observations in its near-infrared channels have been compared to data from a ground-based quasi-global network of Fourier-transform infrared ( FTIR) spectrometers. The SCIAMACHY data considered here have been produced by three different retrieval algorithms, WFM-DOAS (version 0.5 for CO and CH4 and version 0.4 for CO2 and N2O), IMAP- DOAS ( version 1.1 and 0.9 (for CO)) and IMLM (version 6.3) and cover the January to December 2003 time period. Comparisons have been made for individual data, as well as for monthly averages. To maximize the number of reliable coincidences that satisfy the temporal and spatial collocation criteria, the SCIAMACHY data have been compared with a temporal 3rd order polynomial interpolation of the ground-based data. Particular attention has been given to the question whether SCIAMACHY observes correctly the seasonal and latitudinal variability of the target species. The present results indicate that the individual SCIAMACHY data obtained with the actual versions of the algorithms have been significantly improved, but that the quality requirements, for estimating emissions on regional scales, are not yet met. Nevertheless, possible directions for further algorithm upgrades have been identified which should result in more reliable data products in a near future. [less ▲]

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See detailLong-term trend of CH4 at northern mid-latitudes: Comparison between ground-based infrared solar and surface sampling measurements
Rinsland, Curtis P.; Goldman, Aaron; Elkins, James W. et al

in Journal of Quantitative Spectroscopy & Radiative Transfer (2006), 97(3), 457-466

We report average tropospheric CH4 volume mixing ratios retrieved from a 27 year time series of high spectral resolution infrared solar absorption measurements recorded between May 1977 and July 2004 at ... [more ▼]

We report average tropospheric CH4 volume mixing ratios retrieved from a 27 year time series of high spectral resolution infrared solar absorption measurements recorded between May 1977 and July 2004 at the US National Solar Observatory station on Kitt Peak (31.9 degrees N, 111.6 degrees W, 2.09 km altitude) and their comparison with surface in situ sampling measurements recorded between 1983 and 2004 at the Climate Monitoring and Diagnostics Laboratory (CMDL) station at Niwot Ridge, Colorado (40.0 degrees N, 105.5 degrees W, 3013 m altitude). The two measurement sets therefore overlap for the 1983-2004 time period. An average tropospheric volume mixing ratios of 1814 +/- 48 ppbv (1 ppbv = 10(-9) per unit volume) has been derived from the solar absorption time series with a best-fit increase rate trend equal to 8.26 +/- 2.20 ppbv yr(-1) in 1983 decreasing to 1.94 +/- 3.69 ppbv yr(-1) in 2003. The CMDL measurements also show a continuous long-term CH4 volume mixing ratio rise, with subsequent slowing down. A mean ratio of the retrieved average tropospheric volume mixing ratio to the CMDL volume mixing ratio for the overlapping time period of 1.038 +/- 0.034 indicates agreement between both data sets within the quantified experimental errors. (C) 2005 Elsevier Ltd. All rights reserved. [less ▲]

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See detailLong-term stratospheric carbon tetrafluoride (CF4) increase inferred from 1985-2004 infrared space-based solar occultation measurements
Rinsland, Curtis P.; Mahieu, Emmanuel ULg; Zander, Rodolphe ULg et al

in Geophysical Research Letters (2006), 33(2),

The long-term stratospheric carbon tetrafluoride (CF4) increase has been determined from infrared high spectral resolution solar occultation Fourier transform spectrometer measurements between 3 and 50 ... [more ▼]

The long-term stratospheric carbon tetrafluoride (CF4) increase has been determined from infrared high spectral resolution solar occultation Fourier transform spectrometer measurements between 3 and 50 hPa (similar to 20 to 40 km altitude) and latitudes from 50 degrees N to 50 degrees S during 1985, 1992, 1993, 1994, and 2004. The 1985 to 1994 measurements were recorded from the ATMOS ( Atmospheric Trace MOlecule Spectroscopy) instrument at 0.01 cm(-1) resolution and in 2004 by the Atmospheric Chemistry Experiment ( ACE) instrument at 0.02 cm(-1) resolution. Stratospheric volume mixing ratios, inferred from a polynomial fit to averages from the time periods considered here, increased from 49.37 +/- 2.60 pptv (10(-12) per unit volume) in 1985 to 58.38 +/- 4.14 pptv in 1992, 60.46 +/- 2.97 pptv in 1993, 60.11 +/- 3.60 pptv in 1994 and to 70.45 +/- 3.40 pptv in 2004. The stratospheric CF4 mixing ratio has continued to increase but at a slower rate than in previous years, for example, (1.14 +/- 0.68)% yr(-1) in 2004 as compared to (2.77 +/- 0.47)% yr(-1) in 1985, 1 sigma. Correlations of CF4 with N2O taking into account the increase of N2O with time also show the increase in the stratospheric CF4 burden over the two decade measurement time span. Our space-based measurements show that the slowdown in the rate of CF4 accumulation previously reported from surface measurements through 1997 has propagated to the stratosphere and is continuing. Citation: Rinsland, C. P., E. Mahieu, R. Zander, R. Nassar, P. Bernath, C. Boone, and L. S. Chiou (2006), Long-term stratospheric carbon tetrafluoride (CF4) increase inferred from 1985-2004 infrared space-based solar occultation measurements, Geophys. Res. Lett., 33, L02808, doi:10.1029/2005GL024709. [less ▲]

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See detailTrends of HF, HCl, CCl2F2, CCl3F, CHClF2 (HCFC-22), and SF6 in the lower stratosphere from Atmospheric Chemistry Experiment (ACE) and Atmospheric Trace Molecule Spectroscopy (ATMOS) measurements near 30 degrees N latitude
Rinsland, Curtis P.; Boone, Christopher D.; Nassar, Ray et al

in Geophysical Research Letters (2005), 32(16),

[ 1] Volume mixing ratios ( VMRs) of HF, HCl, CCl2F2, CHClF2 ( HCFC-22), and SF6 in the lower stratosphere have been derived from solar occultation measurements recorded with spaceborne high resolution ... [more ▼]

[ 1] Volume mixing ratios ( VMRs) of HF, HCl, CCl2F2, CHClF2 ( HCFC-22), and SF6 in the lower stratosphere have been derived from solar occultation measurements recorded with spaceborne high resolution Fourier transform spectrometers. Atmospheric Chemistry Experiment ( ACE) VMRs measured during 2004 have been compared with those obtained in 1985 and 1994 by the Atmospheric Trace MOlecule Spectroscopy ( ATMOS) instrument. Trends are estimated by referencing the measured VMRs to those of the long-lived constituent N2O to account for variations in the dynamic history of the sampled air masses. Pressure-gridded measurements covering 10-100 hPa ( similar to 16 to 30 km altitude) were used in the analysis that includes typically 25 degrees N-35 degrees N latitude. The VMR changes provide further evidence of the impact of the emission restrictions imposed by the Montreal Protocol and its strengthening amendments and adjustments and are consistent with model predictions and known sources and sinks of halocarbons. Decreases in the lower stratospheric mixing ratios of CCl3F and HCl are measured in 2004 with respect to 1994, providing important confirmation of recent ground-based solar absorption measurements of a decline in inorganic chlorine. Trends estimates are compared with other reported measurements and model predictions. [less ▲]

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