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See detailRecent trend anomaly of hydrogen chloride (HCl) at northern mid-latitudes derived from Jungfraujoch, HALOE and ACE-FTS Infrared solar observations
Mahieu, Emmanuel ULg; Zander, Rodolphe ULg; Bernath, Peter F. et al

in Bernath, Peter F. (Ed.) The Atmospheric Chemistry Experiment ACE at 10: A Solar Occultation Anthology (2013)

In this contribution, we analyze infrared solar observations recorded from the ground at the Jungfraujoch station and from space with the HALOE and the ACE-FTS instruments to derive time series of ... [more ▼]

In this contribution, we analyze infrared solar observations recorded from the ground at the Jungfraujoch station and from space with the HALOE and the ACE-FTS instruments to derive time series of stratospheric columns of hydrogen chloride (HCl) at Northern mid-latitudes. We investigate the Jungfraujoch and the composite satellite time series to characterize the evolution of HCl over the last 15 years, i.e. after its peak loading which occurred in 1996 in this region of the Earth’s atmosphere. Trends derived from both data sets are compared and possible causes for the recent change in the stratospheric HCl buildup are evoked. [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 detailTrend and lifetime of sulfur hexafluoride at mid-latitudes deduced from ACE-FTS occultation measurements
Mahieu, Emmanuel ULg; Duchatelet, Pierre ULg; Zander, Rodolphe ULg et al

in Geophysical Research Abstracts (2011), 13

Sulfur hexafluoride (SF6) is one of the strongest greenhouse gases on a per molecule basis, with a global warming potential of 22800 (100-yr horizon). This is an extremely stable gas in the atmosphere ... [more ▼]

Sulfur hexafluoride (SF6) is one of the strongest greenhouse gases on a per molecule basis, with a global warming potential of 22800 (100-yr horizon). This is an extremely stable gas in the atmosphere, which results in a very long lifetime, with large uncertainties. The value adopted by IPCC is 3200 years, but some studies suggest shorter lifetimes, as low as 800 years. Surface concentrations are now about 7 ppt, with reported trends indicating a steady and strong increase of 0.3 ppt/yr. Most emissions are of anthropogenic origin, related to its use as an insulator in high-voltage electrical installations. Secondary contributions result from magnesium and aluminum production as well as from the manufacturing of semiconductors (see e.g. Levin et al., 2010; Rigby et al., 2010 and references therein). In this contribution, we use occultation measurements performed by the ACE-FTS (Atmospheric Chemistry Experiment Fourier Transform Spectrometer) instrument, launched in August 2003 onboard the Canadian SCISAT satellite (Bernath et al., 2005). ACE-FTS is still in operation to date, with no significant degradation in its performance. This spectrometer achieves a spectral resolution of 0.02 cm-1 in the broad 750-4400 cm-1 range which covers the unresolved nu-3 band Q branch of SF6 centered at 947.9 cm-1. Signal-to-noise ratios of 200-300 are typically obtained in the spectral region of interest. Version 3 retrievals performed by University of Waterloo give volume mixing ratio profiles of SF6 in the 11-32 km altitude range. We consider all available sunrise and sunset occultation measurements obtained at midlatitudes in both hemispheres to derive the trend of SF6 in the lower stratosphere, from late February 2004 onwards. Consistency between both hemispheres will be investigated. In addition, concurrent N2O measurements are used to evaluate the atmospheric lifetime of SF6, following a method used previously for other long-lived gases (e.g. Zander et al, 1996). Comparisons with trends derived from in situ surface measurements or from ground-based remote-sensing observations (e.g. at the Jungfraujoch station, 46.5ºN) are also included. [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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