Two‐dimensional model calculation of fluorine‐containing reservoir species in the stratosphere

Kaye, Jack A.; Douglass, Anne R.; Jackman, Charles H.; Stolarski, R. S.; Zander, Rodolphe; Roland, G.

doi:10.1029/91jd01178

Cited by 46 publications

(50 citation statements)

References 32 publications

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“…The ACE payload, also known as SCISAT-1, was successfully launched on 12 August 2003 into a 74 inclined orbit by a NASA-supplied Pegasus XL at 650 km altitude [13]. This small Canadian-designed and built satellite contains three instruments with a shared field of view, and with the primary goal of recording…”

Section: Measurementsmentioning

confidence: 99%

“…The global distribution of COClF [13] for 1989 was predicted to be relatively symmetric about the equator with the highest VMR of $100 pptv (1 pptv ¼ 10 À12 per unit volume) at 20 hPa. The model distribution showed lower maximum VMRs with peaks shifted to higher pressure levels in both hemispheres for March and June 1989.…”

Section: Introductionmentioning

confidence: 99%

“…Carbonyl chlorofluoride or chlorofluorocarbonyl (COClF), also referred to as CFClO or OCClF, is a reservoir species that results from the breakdown of CCl 3 F [6][7][8][9][10][11][12][13]. It is the most easily photolyzed F-containing breakdown product with a mixing ratio that decreases rapidly above the peak.…”

Section: Introductionmentioning

confidence: 99%

“…It is the most easily photolyzed F-containing breakdown product with a mixing ratio that decreases rapidly above the peak. Modeled COClF assuming a 3% per year increase between 1990 and 1994 was used to estimate stratospheric chlorine from Atmospheric Trace MOlecule Spectroscopy (ATMOS) measurements at northern mid-latitudes (35-491N) and the northern subtropics during 1994 [13]. Production of COClF is analogous to the CH 4 oxidation scheme, and is based on the assumption that in chlorofluorocarbons (CFCs), all C-Cl bonds break before C-F bonds and for HCFCs, C-H bonds break first, followed by C-Cl bonds, and then C-F bonds.…”

Section: Introductionmentioning

confidence: 99%

“…Removal of COClF by Oð 1 DÞ was also accounted for with the modeled COClF distribution reported as a function of latitude and different seasons in 1989 [13]. The global distribution of COClF [13] for 1989 was predicted to be relatively symmetric about the equator with the highest VMR of $100 pptv (1 pptv ¼ 10 À12 per unit volume) at 20 hPa.…”

Section: Introductionmentioning

confidence: 99%

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Spectroscopic detection of COClF in the tropical and mid-latitude lower stratosphere

Rinsland

Nassar

Boone

et al. 2007

Journal of Quantitative Spectroscopy and Radiative Transfer

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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 AE 48:0 pptv (10 À12 per unit volume, 1 sigma) is measured at 28 km for tropical and subtropical occultations (latitudes below 20 in both hemispheres) with lower mixing ratios at both higher and lower altitudes. Northern hemisphere mid-latitude mixing ratios (30-501N) resulted in an average profile with a peak mixing ratio of 51:7 AE 32:1 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. r

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Section: Measurementsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 3 more Smart Citations

Spectroscopic detection of COClF in the tropical and mid-latitude lower stratosphere

Rinsland

Nassar

Boone

et al. 2007

Journal of Quantitative Spectroscopy and Radiative Transfer

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Ozone depletion by hydrofluorocarbons

Hurwitz

Fleming

Newman

et al. 2015

Geophys. Res. Lett.

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Atmospheric concentrations of hydrofluorocarbons (HFCs) are projected to increase considerably in the coming decades. Chemistry climate model simulations forced by current projections show that HFCs will impact the global atmosphere increasingly through 2050. As strong radiative forcers, HFCs increase tropospheric and stratospheric temperatures, thereby enhancing ozone‐destroying catalytic cycles and modifying the atmospheric circulation. These changes lead to a weak depletion of stratospheric ozone. Simulations with the NASA Goddard Space Flight Center 2‐D model show that HFC‐125 is the most important contributor to HFC‐related atmospheric change in 2050; its effects are comparable to the combined impacts of HFC‐23, HFC‐32, HFC‐134a, and HFC‐143a. Incorporating the interactions between chemistry, radiation, and dynamics, ozone depletion potentials (ODPs) for HFCs range from 0.39 × 10−3 to 30.0 × 10−3, approximately 100 times larger than previous ODP estimates which were based solely on chemical effects.

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Supercooled Sulfuric Acid Droplets: Perturbed Stratospheric Chemistry in Early Winter

Turco

Hamill

1992

Ber Bunsenges Phys Chem

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During the onset of polar winter in the stratosphere, before the formation of nitric acid ice clouds (referred to as polar stratospheric clouds, or PSCs), sulfate aerosol particles may catalyze heterogeneous chemical reactions that redistribute chlorine from reservoir species to more active forms. This activated chlorine can lead to ozone destruction in the fall and early winter, prior to the formation of PSCs, at middle and high latitudes over the winter half‐year in both hemispheres. During periods of slow cooling, a significant fraction of ambient chlorine nitrate (ClONO2) may be processed into active chlorine through its reactions with water and HCl at the surfaces of dilute supercooled sulfuric acid droplets. This mechanism for chlorine activation may explain the occurrence of widespread regions of reduced ozone abundance in the Northern Hemisphere at high‐ and middle‐latitudes outside of the polar vortex. Following major volcanic eruptions, a large increase in the surface area of sulfate particles could lead to significant repartitioning of chlorine species via the reaction of ClONO2 with H2O, even under midlatitude conditions, which may explain in part the detection of ozone reductions in volcanic clouds. Chemical transformation of other compounds may also be accelerated by the presence of dilute supercooled sulfate aerosols in the stratosphere, including the reaction of HOCl with HCl, and the hydrolysis of COF2 to HF; however, neither of these latter processes appear to have first‐order significance for the chemistry of the stratosphere.

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Two‐dimensional model calculation of fluorine‐containing reservoir species in the stratosphere

Cited by 46 publications

References 32 publications

Spectroscopic detection of COClF in the tropical and mid-latitude lower stratosphere

Spectroscopic detection of COClF in the tropical and mid-latitude lower stratosphere

Ozone depletion by hydrofluorocarbons

Supercooled Sulfuric Acid Droplets: Perturbed Stratospheric Chemistry in Early Winter

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