scholarly journals The HNO<sub>3</sub> forming branch of the HO<sub>2</sub> + NO reaction: pre-industrial-to-present trends in atmospheric species and radiative forcings

2011 ◽  
Vol 11 (17) ◽  
pp. 8929-8943 ◽  
Author(s):  
O. A. Søvde ◽  
C. R. Hoyle ◽  
G. Myhre ◽  
I. S. A. Isaksen
Keyword(s):  
Radiative Forcing ◽  
Transport Model ◽  
Three Dimensional ◽  
Branching Ratio ◽  
Pressure Effects ◽  
Atmospheric Composition ◽  
Radiative Forcings ◽  
Atmospheric Species ◽  
Tropospheric O3 ◽  
The Tropics

Abstract. Recent laboratory measurements have shown the existence of a HNO3 forming branch of the HO2 + NO reaction. This reaction is the main source of tropospheric O3, through the subsequent photolysis of NO2, as well as being a major source of OH. The branching of the reaction to HNO3 reduces the formation of these species significantly, affecting O3 abundances, radiative forcing and the oxidation capacity of the troposphere. The Oslo CTM2, a three-dimensional chemistry transport model, is used to calculate atmospheric composition and trends with and without the new reaction branch. Results for the present day atmosphere, when both temperature and pressure effects on the branching ratio are accounted for, show an 11 % reduction in the calculated tropospheric burden of O3, with the main contribution from the tropics. An increase of the global, annual mean methane lifetime by 10.9 %, resulting from a 14.1 % reduction in the global, annual mean OH concentration is also found. Comparisons with measurements show that including the new branch improves the modelled O3 in the Oslo CTM2, but that it is not possible to conclude whether the NOy distribution improves. We model an approximately 11 % reduction in the tropical tropospheric O3 increase since pre-industrial times, and a 4 % reduction of the increase in total tropospheric burden. Also, an 8 % decrease in the trend of OH concentrations is calculated, when the new branch is accounted for. The radiative forcing due to changes in O3 over the industrial era was calculated as 0.33 W m−2, reducing to 0.26 W m−2 with the new reaction branch. These results are significant, and it is important that this reaction branching is confirmed by other laboratory groups.

scholarly journals The HNO<sub>3</sub> forming branch of the HO<sub>2</sub> + NO reaction: pre-industrial-to-present trends in atmospheric species and radiative forcings

2011 ◽  
Vol 11 (5) ◽  
pp. 14801-14835 ◽  
Author(s):  
O. A. Søvde ◽  
C. R. Hoyle ◽  
G. Myhre ◽  
I. S. A. Isaksen
Keyword(s):  
Radiative Forcing ◽  
Transport Model ◽  
Three Dimensional ◽  
Branching Ratio ◽  
Pressure Effects ◽  
Atmospheric Composition ◽  
Chemistry Transport Model ◽  
Radiative Forcings ◽  
Atmospheric Species ◽  
Temperature And Pressure Effects

Abstract. Recent laboratory measurements have shown the existence of a HNO3 forming branch of the HO2 + NO reaction. This reaction is the main source of atmospheric O3, through the subsequent photolysis of NO2, as well as being a major source of OH. The branching of the reaction to HNO3 reduces the formation of these species significantly, affecting O3 abundances, climate and the oxidation capacity of the troposphere. The Oslo CTM2, a three-dimensional chemistry transport model, is used to calculate atmospheric composition and trends with and without the new reaction branch. Results for the present day atmosphere, when both temperature and pressure effects on the branching ratio are accounted for, show an increase of the global, annual mean methane lifetime by 10.9 %, resulting from a 14.1 % reduction in the global, annual mean OH concentration. Comparisons with measurements show that including the new branch improves the modelled O3, but that it is not possible to conclude whether the NOy distribution improves. We model an approximately 11 % reduction in the tropical tropospheric O3 increase since pre-industrial times, as well as an 8 % decrease in the trend of OH concentration, when the new branch is accounted for. The radiative forcing due to changes in O3 over the industrial era was calculated as 0.33 W m−2, reducing to 0.26 W m−2 with the new reaction branch. These results are significant, and it is important that this reaction branching is confirmed by other laboratory groups.

scholarly journals Analysis of a rapid increase of stratospheric ozone during late austral summer 2008 over Kerguelen (49.4° S, 70.3° E)

2011 ◽  
Vol 11 (1) ◽  
pp. 363-373 ◽  
Author(s):  
H. Bencherif ◽  
L. El Amraoui ◽  
G. Kirgis ◽  
J. Leclair De Bellevue ◽  
A. Hauchecorne ◽  
...  
Keyword(s):  
Potential Vorticity ◽  
Large Scale ◽  
Lower Stratosphere ◽  
Transport Model ◽  
Stratospheric Ozone ◽  
Three Dimensional ◽  
Austral Summer ◽  
Air Masses ◽  
Global Mapping ◽  
The Tropics

Abstract. This paper reports on an increase of ozone event observed over Kerguelen (49.4° S, 70.3° E) in relationship with large-scale isentropic transport. This is evidenced by ground-based observations (co-localised radiosonde and SAOZ experiments) together with satellite global observations (Aura/MLS) assimilated into MOCAGE, a Méteo-France model. The study is based on the analyses of the first ozonesonde experiment never recorded at the Kerguelen site within the framework of a French campaign called ROCK that took place from April to August 2008. Comparisons and interpretations of the observed event are supported by co-localised SAOZ observations, by global mapping of tracers (O3, N2O and columns of O3) from Aura/MLS and Aura/OMI experiments, and by model simulations of Ertel Potential Vorticity initialised by the ECMWF (European Centre for Medium-Range Weather Forecasts) data reanalyses. Satellite and ground-based observational data revealed a consistent increase of ozone in the local stratosphere by mid-April 2008. Additionally, Ozone (O3) and nitrous oxide (N2O) profiles obtained during January–May 2008 using the Microwave Limb Sounder (MLS) aboard the Aura satellite are assimilated into MOCAGE (MOdèle de Chimie Atmosphérique à Grande Echelle), a global three-dimensional chemistry transport model of Météo-France. The assimilated total O3 values are consistent with SAOZ ground observations (within ±5%), and isentropic distributions of O3 match well with maps of advected potential vorticity (APV) derived from the MIMOSA model, a high-resolution advection transport model, and from the ECMWF reanalysis. The event studied seems to be related to the isentropic transport of air masses that took place simultaneously in the lower- and middle-stratosphere, respectively from the polar region and from the tropics to the mid-latitudes. In fact, the ozone increase observed by mid April 2008 resulted simultaneously: (1) from an equator-ward departure of polar air masses characterised with a high-ozone layer in the lower stratosphere (near the 475 K isentropic level), and (2) from a reverse isentropic transport from the tropics to mid- and high-latitudes in the upper stratosphere (nearby the 700 K level). The increase of ozone observed over Kerguelen from the 16-April ozonesonde profile is thus attributed to a concomitant isentropic transport of ozone in two stratospheric layers: the tropical air moving southward and reaching over Kerguelen in the upper stratosphere, and the polar air passing over the same area but in the lower stratosphere.

scholarly journals Evaluation of near-tropopause ozone distributions in the Global Modeling Initiative combined stratosphere/troposphere model with ozonesonde data

2008 ◽  
Vol 8 (1) ◽  
pp. 1589-1634 ◽  
Author(s):  
D. B. Considine ◽  
J. A. Logan ◽  
M. A. Olsen
Keyword(s):  
Annual Cycle ◽  
Transport Model ◽  
Model Simulation ◽  
Atmospheric Composition ◽  
Vertical Resolution ◽  
Residual Circulation ◽  
Vertical Diffusion ◽  
Global Modeling ◽  
Upper Troposphere ◽  
The Tropics

Abstract. The NASA Global Modeling Initiative has developed a combined stratosphere/troposphere chemistry and transport model which fully represents the processes governing atmospheric composition near the tropopause. We evaluate model ozone distributions near the tropopause, using two high vertical resolution monthly mean ozone profile climatologies constructed with ozonesonde data, one by averaging on pressure levels and the other relative to the thermal tropopause. Model ozone is high-biased at the SH tropical and NH midlatitude tropopause by ~45% in a 4° latitude × 5° longitude model simulation. Increasing the resolution to 2°×2.5&amp;deg increases the NH tropopause high bias to ~60%, but decreases the tropical tropopause bias to ~30%, an effect of a better-resolved residual circulation. The tropopause ozone biases appear not to be due to an overly vigorous residual circulation or excessive stratosphere/troposphere exchange, but are more likely due to insufficient vertical resolution or excessive vertical diffusion near the tropopause. In the upper troposphere and lower stratosphere, model/measurement intercomparisons are strongly affected by the averaging technique. NH and tropical mean model lower stratospheric biases are <20%. In the upper troposphere, the 2°×2.5&amp;deg simulation exhibits mean high biases of ~20% and~35% during April in the tropics and NH midlatitudes, respectively, compared to the pressure-averaged climatology. However, relative-to-tropopause averaging produces upper troposphere high biases of ~30% and 70% in the tropics and NH midlatitudes. This is because relative-to-tropopause averaging better preserves large cross-tropopause O3 gradients, which are seen in the daily sonde data, but not in daily model profiles. The relative annual cycle of ozone near the tropopause is reproduced very well in the model Northern Hemisphere midlatitudes. In the tropics, the model amplitude of the near-tropopause annual cycle is weak. This is likely due to the annual amplitude of mean vertical upwelling near the tropopause, which analysis suggests is ~30% weaker than in the real atmosphere.

scholarly journals Key drivers of ozone change and its radiative forcing over the 21st century

2018 ◽  
Vol 18 (9) ◽  
pp. 6121-6139 ◽  
Author(s):  
Fernando Iglesias-Suarez ◽  
Douglas E. Kinnison ◽  
Alexandru Rap ◽  
Amanda C. Maycock ◽  
Oliver Wild ◽  
...  
Keyword(s):  
Climate Change ◽  
21St Century ◽  
Radiative Forcing ◽  
Climate Model ◽  
Stratospheric Ozone ◽  
Atmospheric Composition ◽  
Climate Conditions ◽  
Radiative Balance ◽  
Radiative Forcings ◽  
Year 2000

Abstract. Over the 21st century changes in both tropospheric and stratospheric ozone are likely to have important consequences for the Earth's radiative balance. In this study, we investigate the radiative forcing from future ozone changes using the Community Earth System Model (CESM1), with the Whole Atmosphere Community Climate Model (WACCM), and including fully coupled radiation and chemistry schemes. Using year 2100 conditions from the Representative Concentration Pathway 8.5 (RCP8.5) scenario, we quantify the individual contributions to ozone radiative forcing of (1) climate change, (2) reduced concentrations of ozone depleting substances (ODSs), and (3) methane increases. We calculate future ozone radiative forcings and their standard error (SE; associated with inter-annual variability of ozone) relative to year 2000 of (1) 33 ± 104 m Wm−2, (2) 163 ± 109 m Wm−2, and (3) 238 ± 113 m Wm−2 due to climate change, ODSs, and methane, respectively. Our best estimate of net ozone forcing in this set of simulations is 430 ± 130 m Wm−2 relative to year 2000 and 760 ± 230 m Wm−2 relative to year 1750, with the 95 % confidence interval given by ±30 %. We find that the overall long-term tropospheric ozone forcing from methane chemistry–climate feedbacks related to OH and methane lifetime is relatively small (46 m Wm−2). Ozone radiative forcing associated with climate change and stratospheric ozone recovery are robust with regard to background climate conditions, even though the ozone response is sensitive to both changes in atmospheric composition and climate. Changes in stratospheric-produced ozone account for ∼ 50 % of the overall radiative forcing for the 2000–2100 period in this set of simulations, highlighting the key role of the stratosphere in determining future ozone radiative forcing.

scholarly journals Evaluation of near-tropopause ozone distributions in the Global Modeling Initiative combined stratosphere/troposphere model with ozonesonde data

2008 ◽  
Vol 8 (9) ◽  
pp. 2365-2385 ◽  
Author(s):  
D. B. Considine ◽  
J. A. Logan ◽  
M. A. Olsen
Keyword(s):  
Annual Cycle ◽  
Transport Model ◽  
Model Simulation ◽  
Atmospheric Composition ◽  
Vertical Resolution ◽  
Residual Circulation ◽  
Global Modeling ◽  
Upper Troposphere ◽  
The Tropics ◽  
Model Measurement

Abstract. The NASA Global Modeling Initiative has developed a combined stratosphere/troposphere chemistry and transport model which fully represents the processes governing atmospheric composition near the tropopause. We evaluate model ozone distributions near the tropopause, using two high vertical resolution monthly mean ozone profile climatologies constructed with ozonesonde data, one by averaging on pressure levels and the other relative to the thermal tropopause. At the tropopause, model ozone is high-biased in the SH tropics and NH midlatitudes by ~45% in a 4° latitude ×5° longitude model simulation. Doubling the resolution to 2°×2.5° increases the NH high bias to ~60%, and reduces the tropical bias to ~30%, apparently due to decreased horizontal transport between the tropics and extratropics in the higher-resolution simulation. These ozone biases do not appear to be due to an overly vigorous residual circulation, insufficient convection, or excessive stratosphere/troposphere exchange, and so may be due to insufficient vertical resolution or excessive vertical diffusion near the tropopause. In the upper troposphere and lower stratosphere, model/measurement intercomparisons are strongly affected by the averaging technique. Compared to the pressure-averaged climatology, NH and tropical mean model lower stratospheric biases are >20%. In the upper troposphere, the 2°×2.5° simulation shows mean high biases of ~20% and ~35% during April in the tropics and NH midlatitudes, respectively. This apparently good model/measurement agreement degrades when relative-to-tropopause averages are considered, with upper troposphere high biases of ~30% and 70% in the tropics and NH midlatitudes. This occurs because relative-to-tropopause averaging better preserves the larger cross-tropopause O3 gradients which are seen in the daily sonde data, but not in daily model profiles. Relative-to-tropopause averages therefore more accurately reveal model/measurement discrepancies. The relative annual cycle of ozone near the tropopause is reproduced very well in the model Northern Hemisphere midlatitudes. In the tropics, the model amplitude of the near-tropopause annual cycle is weak. This is likely due to the annual amplitude of mean vertical upwelling near the tropopause, which analysis suggests is ~30% weaker than in the real atmosphere.

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

2014 ◽  
Vol 14 (1) ◽  
pp. 267-282 ◽  
Author(s):  
A. T. Brown ◽  
M. P. Chipperfield ◽  
N. A. D. Richards ◽  
C. Boone ◽  
P. F. Bernath
Keyword(s):  
Atmospheric Chemistry ◽  
Radiative Forcing ◽  
Transport Model ◽  
Similar Rate ◽  
Montreal Protocol ◽  
Negative Slope ◽  
Mixing Ratios ◽  
Inorganic Species ◽  
The Tropics ◽  
The Impact

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. The budgets are calculated between 2004 and 2009 for a number of latitude bands: 70–30° N, 30–00° N, 00° N–30° S, and 30–70° S. At lower altitudes total fluorine profiles are dominated by the contribution from CFC-12, up to an altitude of 20 km in the extra-tropics and 29 km in the tropics; above these altitudes the profiles are dominated by hydrogen fluoride (HF). Our data show that total fluorine profiles at all locations have a negative slope with altitude, providing evidence that overall fluorine emissions (measured by their F content) have been increasing with time. 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.

scholarly journals Satellite observations of stratospheric carbonyl fluoride

2014 ◽  
Vol 14 (12) ◽  
pp. 18127-18180 ◽  
Author(s):  
J. J. Harrison ◽  
M. P. Chipperfield ◽  
A. Dudhia ◽  
S. Cai ◽  
S. Dhomse ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Thermal Emission ◽  
Transport Model ◽  
Michelson Interferometer ◽  
Three Dimensional ◽  
Chemical Transport Model ◽  
Northern Latitudes ◽  
Stratospheric Dynamics ◽  
The Tropics ◽  
Carbonyl Fluoride

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).

scholarly journals Bromoform and dibromomethane in the tropics: a 3-D model study of chemistry and transport

2010 ◽  
Vol 10 (2) ◽  
pp. 719-735 ◽  
Author(s):  
R. Hossaini ◽  
M. P. Chipperfield ◽  
B. M. Monge-Sanz ◽  
N. A. D. Richards ◽  
E. Atlas ◽  
...  
Keyword(s):  
Transport Model ◽  
Three Dimensional ◽  
Vertical Motion ◽  
Chemical Transport Model ◽  
Heating Rates ◽  
Tropical Tropopause Layer ◽  
Tropical Tropopause ◽  
Modelling Studies ◽  
Vertical Winds ◽  
The Tropics

Abstract. We have developed a detailed chemical scheme for the degradation of the short-lived source gases bromoform (CHBr3) and dibromomethane (CH2Br2) and implemented it in the TOMCAT/SLIMCAT three-dimensional (3-D) chemical transport model (CTM). The CTM has been used to predict the distribution of the two source gases (SGs) and 11 of their organic product gases (PGs). These first global calculations of the organic PGs show that their abundance is small. The longest lived organic PGs are CBr2O and CHBrO, but their peak tropospheric abundance relative to the surface volume mixing ratio (vmr) of the SGs is less than 5%. We calculate their mean local tropospheric lifetimes in the tropics to be ~7 and ~2 days (due to photolysis), respectively. Therefore, the assumption in previous modelling studies that SG degradation leads immediately to inorganic bromine seems reasonable. We have compared observed tropical SG profiles from a number of aircraft campaigns with various model experiments. In the tropical tropopause layer (TTL) we find that the CTM run using p levels (TOMCAT) and vertical winds from analysed divergence overestimates the abundance of CH2Br2, and to a lesser extent CHBr3, although the data is sparse and comparisons are not conclusive. Better agreement in the TTL is obtained in the sensitivity run using θ levels (SLIMCAT) and vertical motion from diabatic heating rates. Trajectory estimates of residence times in the two model versions show slower vertical transport in the SLIMCAT θ-level version. In the p-level model even when we switch off convection we still find significant amounts of the SGs considered may reach the cold point tropopause; the stratospheric source gas injection (SGI) is only reduced by ~16% for CHBr3 and ~2% for CH2Br2 without convection. Overall, the relative importance of the SG pathway and the PG pathway for transport of bromine to the stratospheric overworld (θ>380 K) has been assessed. Assuming a 10-day washout lifetime of Bry in TOMCAT, we find the delivery of total Br from CHBr3 to be 0.72 pptv with ~53% of this coming from SGI. Similary, for CH2Br2 we find a total Br value of 1.69 pptv with ~94% coming from SGI. We infer that these species contribute ~2.4 pptv of inorganic bromine to the lower stratosphere with SGI being the dominant pathway. Slower transport to and through the TTL would decrease this estimate.

scholarly journals Net radiative forcing and air quality responses to regional CO emission reductions

2012 ◽  
Vol 12 (12) ◽  
pp. 33443-33488
Author(s):  
M. M. Fry ◽  
M. D. Schwarzkopf ◽  
Z. Adelman ◽  
V. Naik ◽  
W. J. Collins ◽  
...  
Keyword(s):  
Air Quality ◽  
Radiative Forcing ◽  
Transport Model ◽  
Surface Ozone ◽  
Ozone Production ◽  
Radiative Transfer Model ◽  
Transfer Model ◽  
International Climate Agreements ◽  
The Tropics ◽  
Reduction Region

Abstract. Carbon monoxide (CO) emissions influence global and regional air quality and global climate change by affecting atmospheric oxidants and secondary species. We simulate the influence of halving anthropogenic CO emissions globally and individually from 10 regions on surface and tropospheric ozone, methane, and aerosol concentrations using a global chemical transport model (MOZART-4 for the year 2005). Net radiative forcing (RF) is then estimated using the GFDL standalone radiative transfer model. We estimate that halving global CO emissions decreases global annual average concentrations of surface ozone by 0.45 ppbv, tropospheric methane by 73 ppbv, and global annual net RF by 36.1 mW m−2, nearly equal to the sum of changes from the 10 regional reductions. Global annual net RF per unit change in emissions and the 100-yr global warming potential (GWP100) are estimated as −0.124 mW m−2 (Tg CO yr−1)−1 and 1.34, respectively, for the global CO reduction, and ranging from −0.115 to −0.131 mW m−2 (Tg CO yr−1)−1 and 1.26 to 1.44 across 10 regions, with the greatest sensitivities for regions in the tropics. The net RF distributions show widespread cooling corresponding to the O3 and CH4 decreases, and localized positive and negative net RFs due to changes in aerosols. The strongest annual net RF impacts occur within the tropics (28° S–28° N) followed by the northern mid-latitudes (28° N–60° N), independent of reduction region, while the greatest changes in surface CO and ozone concentrations occur within the reduction region. Some regional reductions strongly influence the air quality in other regions, such as East Asia, which has an impact on US surface ozone that is 93% of that from North America. Changes in the transport of CO and downwind ozone production clearly exceed the direct export of ozone from each reduction region. The small variation in CO GWPs among world regions suggests that future international climate agreements could adopt a globally uniform metric for CO with little error, or could use different GWPs for each continent. Doing so may increase the incentive to reduce CO through coordinated policies addressing climate and air quality.

scholarly journals Satellite observations of stratospheric carbonyl fluoride

2014 ◽  
Vol 14 (21) ◽  
pp. 11915-11933 ◽  
Author(s):  
J. J. Harrison ◽  
M. P. Chipperfield ◽  
A. Dudhia ◽  
S. Cai ◽  
S. Dhomse ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Thermal Emission ◽  
Transport Model ◽  
Michelson Interferometer ◽  
Three Dimensional ◽  
Chemical Transport Model ◽  
Northern Latitudes ◽  
Stratospheric Dynamics ◽  
The Tropics ◽  
Carbonyl Fluoride

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 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 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 (MIPAS), 0.30 ± 0.44 (ACE), and 0.88% year−1 (SLIMCAT).

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