Modeling the effect of denitrification on Arctic ozone depletion during winter 1999/2000

[1] We have used the SLIMCAT three-dimensional chemical transport model together with observations from the Stratospheric Aerosol and Gas Experiment (SAGE III) Ozone Loss and Validation Experiment (SOLVE) and the Third European Stratospheric Experiment on Ozone (THESEO 2000) to quantify the effect of denitrification on Arctic ozone loss. We have used two different denitrification schemes in the model: one based on the sedimentation of ice particles containing cocondensed nitric acid trihydrate (NAT) and the other based on large NAT particles. The model was forced using both UK Meteorological Office (UKMO) and European Centre for Medium-Range Weather Forecasts (ECMWF) analyses. In the Arctic lower stratosphere the UKMO analyzed temperatures are similar to the ECMWF, except at temperatures near the ice point where the UKMO analyses are colder by over 2 K. Consequently, the UKMO analyses predicted large regions of ice clouds, in contrast to the ECMWF. The denitrification scheme based on large NAT particles gives the best agreement with ER-2 NOy observations for both sets of meteorological analyses. Although the ice scheme and UKMO analyses also produce denitrification, the vertical extent of denitrification and renitrification does not agree as well with the observed NOy. Uncertainties in the budget of ClOy observations from the ER-2 prevent an indirect validation of the best model denitrification scheme based on these data. The denitrified model runs give the best agreement with the observed HCl and ClONO2 reservoirs in mid March. However, UKMO-forced runs generally overestimate the observed ClOx during the same period. The denitrified model runs indicate that by late March 56–74% O3 loss had occurred at 460 K and that denitrification contributed 21–30% of this loss. The model runs showing the largest O3 depletion (forced by UKMO analyses) agree well with ER-2 and ozone sonde data, although these runs overestimated ClOx.

[1]  M. Chipperfield,et al.  A vortex‐scale simulation of the growth and sedimentation of large nitric acid hydrate particles , 2002 .

[2]  D. Fahey,et al.  Observational evidence for the role of denitrification in Arctic stratospheric ozone loss , 2001 .

[3]  T. L. Thompson,et al.  The Detection of Large HNO3-Containing Particles in the Winter Arctic Stratosphere , 2001, Science.

[4]  M. Guirlet,et al.  Large loss of total ozone during the Arctic winter of 1999/2000 , 2000 .

[5]  M. Santee,et al.  UARS Microwave Limb Sounder observations of denitrification and ozone loss in the 2000 Arctic late winter , 2000 .

[6]  M. Chipperfield,et al.  Modeled Arctic ozone depletion in winter 1997/1998 and comparison with previous winters , 2000 .

[7]  G. Manney,et al.  Development of the polar vortex in the 1999–2000 Arctic winter stratosphere , 2000 .

[8]  Santee,et al.  Quantifying denitrification and its effect on ozone recovery , 2000, Science.

[9]  Martyn P. Chipperfield,et al.  The effects of mixing on tracer relationships in the polar vortices , 2000 .

[10]  D. B. Considine,et al.  A polar stratospheric cloud parameterization for the global modeling initiative three-dimensional model and its response to stratospheric aircraft , 2000 .

[11]  Y. Kondo,et al.  Denitrification and nitrification in the Arctic stratosphere during the winter of 1996–1997 , 2000 .

[12]  K. K. Perkins,et al.  The coupling of ClONO2, ClO, and NO2 in the lower stratosphere from in situ observations using the NASA ER‐2 aircraft , 1999 .

[13]  S. Pawson,et al.  The cold winters of the middle 1990s in the northern lower stratosphere , 1999 .

[14]  M. Santee,et al.  Satellite observations of temporary and irreversible denitrification , 1999 .

[15]  Y. Sasano,et al.  NOy-N2O correlation observed inside the Arctic vortex in February 1997 : Dynamical and chemical effects , 1999 .

[16]  L. Froidevaux,et al.  Six years of UARS Microwave Limb Sounder HNO3 observations: Seasonal, interhemispheric, and interannual variations in the lower stratosphere , 1999 .

[17]  A. Ravishankara,et al.  Reconsideration of the rate constant for the reaction of hydroxyl radicals with nitric acid , 1999 .

[18]  P. Crutzen,et al.  Arctic ozone loss due to denitrification , 1999, Science.

[19]  M. Chipperfield,et al.  Ozone depletion at the edge of the Arctic polar vortex 1996/1997 , 1999 .

[20]  Martyn P. Chipperfield,et al.  Multiannual simulations with a three‐dimensional chemical transport model , 1999 .

[21]  A. Ravishankara,et al.  Rate constants for the reaction OH+NO2+M → HNO3+M under atmospheric conditions , 1999 .

[22]  R. Salawitch,et al.  Laminae in the tropical middle stratosphere: Origin and age estimation , 1998 .

[23]  D. McKenna,et al.  Ozone loss rates in the Arctic stratosphere in the winter 1991/92: Model calculations compared with match results , 1998 .

[24]  M. Chipperfield,et al.  Model sensitivity studies of Arctic ozone depletion , 1998 .

[25]  L. Froidevaux,et al.  UARS Microwave Limb Sounder HNO3 observations: Implications for Antarctic polar stratospheric clouds , 1998 .

[26]  M. Danilin,et al.  Stratospheric cooling and arctic ozone recovery , 1998 .

[27]  David Rind,et al.  Increased polar stratospheric ozone losses and delayed eventual recovery owing to increasing greenhouse-gas concentrations , 1998, Nature.

[28]  G. Dutton,et al.  Dehydration and denitrification in the Arctic Polar Vortex during the 1995–1996 winter , 1998 .

[29]  M. Rummukainen,et al.  Prolonged stratospheric ozone loss in the 1995–96 Arctic winter , 1997, Nature.

[30]  P. Rasch,et al.  A three-dimensional simulation of the Antarctic ozone hole: Impact of anthropogenic chlorine on the lower stratosphere and upper troposphere , 1997 .

[31]  S. Pullen,et al.  Accuracy of temperatures from UKMO analyses of 1994/95 in the Arctic winter stratosphere , 1997 .

[32]  B. Knudsen Accuracy of Arctic stratospheric temperature analyses and the implications for the prediction of polar stratospheric clouds , 1996 .

[33]  R. Garcia,et al.  Role of aerosol variations in anthropogenic ozone depletion in the polar regions , 1996 .

[34]  James M. Russell,et al.  Analysis of UARS data in the southern polar vortex in September 1992 using a chemical transport model , 1996 .

[35]  David R. Hanson,et al.  Reaction of BrONO2 with H2O on submicron sulfuric acid aerosol and the implications for the lower stratosphere , 1996 .

[36]  R. Stolarski,et al.  Interhemispheric differences in springtime production of HCl and ClONO2 in the polar vortices , 1995 .

[37]  B. Luo,et al.  An analytic expression for the composition of aqueous HNO3‐H2SO4 stratospheric aerosols including gas phase removal of HNO3 , 1995 .

[38]  P. Brimblecombe,et al.  A Thermodynamic Model of the System HCl-HNO3-H2SO4-H2O, Including Solubilities of HBr, from <200 to 328 K , 1995 .

[39]  L. Froidevaux,et al.  Interhemispheric Differences in Polar Stratospheric HNO3, H2O, CIO, and O3 , 1995, Science.

[40]  B. Luo,et al.  vapour pressures of H2SO4/HNO3/HCl/HBr/H2O solutions to low stratospheric temperatures , 1995 .

[41]  D. R. Hanson,et al.  Reactive Uptake of ClONO2 onto Sulfuric Acid Due to Reaction with HCl and H2O , 1994 .

[42]  Richard Swinbank,et al.  A Stratosphere-Troposphere Data Assimilation System , 1994 .

[43]  R. May,et al.  Aircraft (ER-2) laser infrared absorption spectrometer (ALIAS) for in-situ stratospheric measurements of HCI, N(2)O, CH(4), NO(2), and HNO(3). , 1994, Applied optics.

[44]  S. Wofsy,et al.  Chemical Loss of Ozone in the Arctic Polar Vortex in the Winter of 1991-1992 , 1993, Science.

[45]  D. Fahey,et al.  The Potential for Ozone Depletion in the Arctic Polar Stratosphere , 1991, Science.

[46]  K.,et al.  The Meteorological Measurement System on the NASA ER-2 Aircraft , 1990 .

[47]  S. Solomon,et al.  A diagnostic for denitrification in the winter polar stratospheres , 1990, Nature.

[48]  S. Wofsy,et al.  Loss of ozone in the Arctic vortex for the winter of 1989 , 1990 .

[49]  D. Fahey,et al.  Redistribution of reactive odd nitrogen in the lower arctic stratosphere , 1990 .

[50]  David W. Fahey,et al.  Measurements of nitric oxide and total reactive nitrogen in the Antarctic stratosphere: Observations and chemical implications , 1989 .

[51]  David R. Hanson,et al.  Laboratory studies of the nitric acid trihydrate: Implications for the south polar stratosphere , 1988 .

[52]  M. Molina,et al.  Production of Cl2O2 from the self-reaction of the ClO radical , 1987 .

[53]  M. Prather Numerical advection by conservation of second-order moments. [for trace element spatial distribution and chemical interaction in atmosphere] , 1986 .

[54]  S. Solomon,et al.  On the depletion of Antarctic ozone , 1986, Nature.

[55]  M. Molina,et al.  Chemical kinetics and photochemical data for use in stratospheric modeling , 1985 .

[56]  J. Gras,et al.  On the vapor pressure of sulfuric acid , 1980 .

[57]  J. Noxon Stratospheric NO2 in the Antarctic winter , 1978 .

[58]  F. W. Murray,et al.  On the Computation of Saturation Vapor Pressure , 1967 .