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

Brown, A. T.; Chipperfield, Martyn P.; Richards, N. A. D.; Boone, Christopher D.; Bernath, P. F.

doi:10.5194/acp-14-267-2014

Cited by 11 publications

(18 citation statements)

References 20 publications

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“…Detailed validation studies for HALOE HF measurements were published by Russell III et al (1996). Note that for internal consistency with previous work on the fluorine budget (Brown et al, 2014) and COF 2 (Harrison et al, 2014), the vertical pressure grid has been interpolated onto the standard 1 km grid used by the ACE-FTS.…”

Section: Haloementioning

confidence: 99%

“…Overall the amount of HF in the atmosphere is increasing (e.g. Brown et al, 2014). The first detection of HF in the Earth's stratosphere, based on solar spectra recorded from balloon and on the ground at Jungfraujoch, was made by Zander et al (1977).…”

mentioning

confidence: 99%

“…At the top of the stratosphere most of the fluorine is present as HF (Brown et al, 2014), the dominant reservoir of stratospheric fluorine due to its extreme stability. Note that due to this stability, F is not important for catalytic stratospheric ozone loss.…”

mentioning

confidence: 99%

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Satellite observations of stratospheric hydrogen fluoride and comparisons with SLIMCAT calculations

et al. 2016

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Abstract. The vast majority of emissions of fluorinecontaining molecules are anthropogenic in nature, e.g. chlorofluorocarbons (CFCs), hydrochlorofluorocarbons (HCFCs), and hydrofluorocarbons (HFCs). Many of these fluorine-containing species deplete stratospheric ozone and are regulated by the Montreal Protocol. Once in the atmosphere they slowly degrade, ultimately leading to the formation of hydrogen fluoride (HF), the dominant reservoir of stratospheric fluorine due to its extreme stability. Monitoring the growth of stratospheric HF is therefore an important marker for the success of the Montreal Protocol.We report the comparison of global distributions and trends of HF measured in the Earth's atmosphere by the satellite remote-sensing instruments ACE-FTS (Atmospheric Chemistry Experiment Fourier transform spectrometer), which has been recording atmospheric spectra since 2004, and HALOE (HALogen Occultation Experiment), which recorded atmospheric spectra between 1991 and 2005, with the output of SLIMCAT, a state-of-the-art threedimensional chemical transport model. In general the agreement between observation and model is good, although the ACE-FTS measurements are biased high by ∼ 10 % relative to HALOE. The observed global HF trends reveal a substantial slowing down in the rate of increase of HF since the 1990s: 4.97 ± 0.12 % year −1 (1991-1997; HALOE), 1.12 ± 0.08 % year −1 (1998 HALOE), and 0.52 ± 0.03 % year −1 (2004-2012 ACE-FTS). In comparison, SLIMCAT calculates trends of 4.01, 1.10, and 0.48 % year −1 , respectively, for the same periods; the agreement is very good for all but the earlier of the two HALOE periods. Furthermore, the observations reveal variations in the HF trends with latitude and altitude; for example, between 2004 and 2012 HF actually decreased in the Southern Hemisphere below ∼ 35 km. An additional SLIMCAT simulation with repeating meteorology for the year 2000 produces much cleaner trends in HF with minimal variations with latitude and altitude. Therefore, the variations with latitude and altitude in the observed HF trends are due to variability in stratospheric dynamics on the timescale of a few years. Overall, the agreement between observation and model points towards the ongoing success of the Montreal Protocol and the usefulness of HF as a metric for stratospheric fluorine.

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Section: Haloementioning

confidence: 99%

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confidence: 99%

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Satellite observations of stratospheric hydrogen fluoride and comparisons with SLIMCAT calculations

et al. 2016

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“…Most fluorine in the troposphere is present in its emitted "organic" form due to these molecules having typical lifetimes of a decade or longer; however photolysis in the stratosphere -which liberates fluorine atoms that react with methane, water, or molecular hydrogen -results in the formation of the "inorganic" product hydrogen fluoride, HF. At the top of the stratosphere (∼ 50 km altitude), ∼ 75 % of the total available fluorine is present as HF (Brown et al, 2014). Due to its extreme stability, HF is an almost permanent reservoir of stratospheric fluorine, meaning the atmospheric concentrations of F and Published by Copernicus Publications on behalf of the European Geosciences Union.…”

Section: Introductionmentioning

confidence: 99%

Satellite observations of stratospheric carbonyl fluoride

Harrison¹,

Chipperfield²,

Dudhia³

et al. 2014

Preprint

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Abstract. The vast majority of emissions of fluorine-containing molecules are anthropogenic in nature, e.g. chlorofluorocarbons (CFCs), hydrochlorofluorocarbons (HCFCs), and hydrofluorocarbons (HFCs). These molecules slowly degrade in the atmosphere leading to the formation of HF, COF2, and COClF, which are the main fluorine-containing species in the stratosphere. Ultimately both COF2 and COClF further degrade to form HF, an almost permanent reservoir of stratospheric fluorine due to its extreme stability. Carbonyl fluoride (COF2) is the second most abundant stratospheric "inorganic" fluorine reservoir with main sources being the atmospheric degradation of CFC-12 (CCl2F2), HCFC-22 (CHF2Cl), and CFC-113 (CF2ClCFCl2). This work reports the first global distributions of carbonyl fluoride in the Earth's atmosphere using infrared satellite remote-sensing measurements by the Atmospheric Chemistry Experiment Fourier transform spectrometer (ACE-FTS), which has been recording atmospheric spectra since 2004, and the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) instrument, which has recorded thermal emission atmospheric spectra between 2002 and 2012. The observations reveal a high degree of seasonal and latitudinal variability over the course of a year. These have been compared with the output of SLIMCAT, a state-of-the-art three-dimensional chemical transport model. In general the observations agree well with each other and compare well with SLIMCAT, although MIPAS is biased high by as much as ~30%. Between January 2004 and September 2010 COF2 grew most rapidly at altitudes above ~25 km in the southern latitudes and at altitudes below ~25 km in the northern latitudes, whereas it declined most rapidly in the tropics. These variations are attributed to changes in stratospheric dynamics over the observation period. The overall COF2 global trend over this period is calculated as 0.85 ± 0.34 % year−1 (MIPAS), 0.30 ± 0.44% year−1 (ACE), and 0.88% year−1 (SLIMCAT).

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“…HF is removed from the stratosphere by slow transport to, and rainout in, the troposphere, or by upward transport to the mesosphere, where it is destroyed by photolysis (Duchatelet et al, 2010). The recent stratospheric fluorine inventory for -2009(Brown et al, 2014 indicates a year-on-year increase of HF and total fluorine.…”

Section: J J Harrison Et Al: Satellite Observations Of Stratosphermentioning

confidence: 99%

Satellite observations of stratospheric carbonyl fluoride

et al. 2014

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Abstract. The vast majority of emissions of fluorinecontaining molecules are anthropogenic in nature, e.g. chlorofluorocarbons (CFCs), hydrochlorofluorocarbons (HCFCs), and hydrofluorocarbons (HFCs). These molecules slowly degrade in the atmosphere, leading to the formation of HF, COF 2 , and COClF, which are the main fluorinecontaining species in the stratosphere. Ultimately both COF 2 and COClF further degrade to form HF, an almost permanent reservoir of stratospheric fluorine due to its extreme stability. Carbonyl fluoride (COF 2 ) is the secondmost abundant stratospheric "inorganic" fluorine reservoir, with main sources being the atmospheric degradation of CFC-12 (CCl 2 F 2 ), HCFC-22 (CHF 2 Cl), and CFC-113 (CF 2 ClCFCl 2 ).This work reports the first global distributions of carbonyl fluoride in the Earth's atmosphere using infrared satellite remote-sensing measurements by the Atmospheric Chemistry Experiment Fourier transform spectrometer (ACE-FTS), which has been recording atmospheric spectra since 2004, and the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) instrument, which recorded thermal emission atmospheric spectra between 2002 and 2012. The observations reveal a high degree of seasonal and latitudinal variability over the course of a year. These have been compared with the output of SLIMCAT, a state-of-the-art three-dimensional chemical transport model. In general the observations agree well with each other, although MIPAS is biased high by as much as ∼ 30 %, and compare well with SLIMCAT.Between January 2004 and September 2010 COF 2 grew most rapidly at altitudes above ∼ 25 km in the southern latitudes and at altitudes below ∼ 25 km in the northern latitudes, whereas it declined most rapidly in the tropics. These variations are attributed to changes in stratospheric dynamics over the observation period. The overall COF 2 global trend over this period is calculated as 0.85 ± 0.34 (MIPAS), 0.30 ± 0.44 (ACE), and 0.88 % year −1 (SLIMCAT).

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

Cited by 11 publications

References 20 publications

Satellite observations of stratospheric hydrogen fluoride and comparisons with SLIMCAT calculations

Satellite observations of stratospheric hydrogen fluoride and comparisons with SLIMCAT calculations

Satellite observations of stratospheric carbonyl fluoride

Satellite observations of stratospheric carbonyl fluoride

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