The 1985 chlorine and fluorine inventories in the stratosphere based on ATMOS observations at 30� north latitude

Zander, Rodolphe; Gunson, M. R.; Farmer, C. B.; Rinsland, C. P.; Irion, F. W.; Mahieu, Emmanuel

doi:10.1007/bf00053758

Cited by 92 publications

(75 citation statements)

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“…Decomposition of chlorine-containing source gases (SG Cl ) in the stratosphere produces HCl, the largest reservoir of chlorine 8,9 . Here we investigate recent trends in atmospheric We are grateful to all colleagues who have contributed to FTIR data acquisition.…”

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confidence: 99%

Recent Northern Hemisphere stratospheric HCl increase due to atmospheric circulation changes

Mahieu

Chipperfield

Notholt

et al. 2014

Nature

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The abundance of chlorine in the Earth's atmosphere increased considerably during the 1970s to 1990s, following large emissions of anthropogenic long-lived chlorine-containing source gases, notably the chlorofluorocarbons. The chemical inertness of chlorofluorocarbons allows their transport and mixing throughout the troposphere on a global scale1, before they reach the stratosphere where they release chlorine atoms that cause ozone depletion2. The large ozone loss over Antarctica3 was the key observation that stimulated the definition and signing in 1987 of the Montreal Protocol, an international treaty establishing a schedule to reduce the production of the major chlorine-and bromine-containing halocarbons. Owing to its implementation, the near-surface total chlorine concentration showed a maximum in 1993, followed by a decrease of half a per cent to one per cent per year4, in line with expectations. Remote-sensing data have revealed a peak in stratospheric chlorine after 19965, then a decrease of close to one per cent per year6, 7, in agreement with the surface observations of the chlorine source gases and model calculations7. Here we present ground-based and satellite data that show a recent and significant increase, at the 2σ level, in hydrogen chloride (HCl), the main stratospheric chlorine reservoir, starting around 2007 in the lower stratosphere of the Northern Hemisphere, in contrast with the ongoing monotonic decrease of near-surface source gases. Using model simulations, we attribute this trend anomaly to a slowdown in the Northern Hemisphere atmospheric circulation, occurring over several consecutive years, transporting more aged air to the lower stratosphere, and characterized by a larger relative conversion of source gases to HCl. This short-term dynamical variability will also affect other stratospheric tracers and needs to be accounted for when studying the evolution of the stratospheric ozone layer. Disciplines Medicine and Health Sciences | Social and Behavioral Sciences Publication DetailsMahieu, E., Chipperfield, M. P., Notholt, J., Reddmann, T., Anderson, J., Bernath, P. F., Blumenstock, T., Coffey, M. T., Dhomse, S. S., Feng, W., Franco, B., Froidevaux, L., Griffith, D. W. T., Hannigan, J. W., Hase, F., Hossaini, R., Jones, N. B., Morino, I., Murata, I., Nakajima, H., Palm, M., Paton-Walsh, C., Russell III, J. M., Schneider, M., Servais, C., Smale, D. & Walker, K. A. (2014). Recent Northern Hemisphere stratospheric HCl increase due to atmospheric circulation changes. Nature, 515 (7525), 104-107. The large ozone loss over Antarctica 3 was the key observation which stimulated the definition and signing of the Montreal Protocol in 1987, an international treaty establishing a schedule to reduce the production of the major chlorine-and brominecontaining halocarbons. Owing to its implementation, the near-surface total chlorine concentration showed a maximum in 1993, followed by a decrease of 0.5-1 %/yr 4 , in line with expectations. Remote-sensing data have revealed a peak in stratospheric...

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confidence: 99%

Recent Northern Hemisphere stratospheric HCl increase due to atmospheric circulation changes

Mahieu

Chipperfield

Notholt

et al. 2014

Nature

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113

112

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“…A number of fluorine budgets have been calculated previously. Measurements made by the Atmospheric Trace Molecule Spectroscopy (ATMOS) instrument were used to calculate a stratospheric fluorine budget using VMR profiles of CF 4 , CFC-11, CFC-12, COF 2 , HCFC-22, HF and SF 6 at 30 • N for 1985 (Zander et al, 1992). Further work was carried out using the Jet Propulsion Laboratory's MkIV balloon-borne Fourier transform spectrometer retrievals of CF 4 , CFC-11, CFC-12, CFC-113, COF 2 , HCFC-22, HF and SF 6 (Sen et al, 1996).…”

Section: Speciesmentioning

confidence: 99%

Global stratospheric fluorine inventory for 2004–2009 from Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) measurements and SLIMCAT model simulations

et al. 2014

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Abstract. Fluorine-containing species can be extremely effective atmospheric greenhouse gases. We present fluorine budgets using organic and inorganic species retrieved by the ACE-FTS satellite instrument supplemented with output from the SLIMCAT 3-D chemical transport model Total stratospheric fluorine is increasing at a similar rate in the tropics: 32.5 ± 4.9 ppt yr −1 (1.31 ± 0.20 % per year) in the Northern Hemisphere (NH) and 29.8 ± 5.3 ppt yr −1 (1.21 ± 0.22 % per year) in the Southern Hemisphere (SH). Extra-tropical total stratospheric fluorine is also increasing at a similar rate in both the NH and SH: 28.3 ± 2.7 ppt per year (1.12 ± 0.11 % per year) in the NH and 24.3 ± 3.1 ppt per year (0.96 ± 0.12 % per year) in the SH. The calculation of radiative efficiency-weighted total fluorine allows the changes in radiative forcing between 2004 and 2009 to be calculated. These results show an increase in radiative forcing of between 0.23 ± 0.11 % per year and 0.45 ± 0.11 % per year, due to the increase in fluorine-containing species during this time. The decreasing trends in the mixing ratios of halons and chlorofluorocarbons (CFCs), due to their prohibition under the Montreal Protocol, have suppressed an increase in total fluorine caused by increasing mixing ratios of hydrofluorocarbons (HFCs). This has reduced the impact of fluorine-containing species on global warming.

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“…Knowledge of the distribution of inorganic chlorine Cl y in the stratosphere is needed to attribute changes in stratospheric ozone to changes in halogens, and to assess the realism of chemistry-climate models (Eyring et al, 2006, Eyring et al, 2007, Waugh and Eyring, 2008. However, simultaneous measurements of the major inorganic chlorine species are rare (Zander et al, 1992, Webster et al, 1994, Sen et al, 1999, Bonne et al, 2000, Voss et al, 2001. In the upper stratosphere, the situation is a little easier as Cl y can be inferred from HCl alone (e.g., , Froidevaux et al, 2006b, Santee et al, 2008).…”

Section: Bias Correction: Atmospheric Chlorine Loading For Ozone Holementioning

confidence: 99%

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The 1985 chlorine and fluorine inventories in the stratosphere based on ATMOS observations at 30� north latitude

Cited by 92 publications

References 44 publications

Recent Northern Hemisphere stratospheric HCl increase due to atmospheric circulation changes

Recent Northern Hemisphere stratospheric HCl increase due to atmospheric circulation changes

Global stratospheric fluorine inventory for 2004–2009 from Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) measurements and SLIMCAT model simulations

Artificial Intelligence in Aerospace

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