Simulation of polar ozone depletion: An update

We evaluate polar ozone depletion chemistry using the specified dynamics version of the Whole Atmosphere Community Climate Model for the year 2011. We find that total ozone depletion in both hemispheres is dependent on cold temperatures (below 192 K) and associated heterogeneous chemistry on polar stratospheric cloud particles. Reactions limited to warmer temperatures above 192 K, or on binary liquid aerosols, yield little modeled polar ozone depletion in either hemisphere. An imposed factor of three enhancement in stratospheric sulfate increases ozone loss by up to 20 Dobson unit (DU) in the Antarctic and 15 DU in the Arctic in this model. Such enhanced sulfate loads are similar to those observed following recent relatively small volcanic eruptions since 2005 and imply impacts on the search for polar ozone recovery. Ozone losses are strongly sensitive to temperature, with a test case cooler by 2 K producing as much as 30 DU additional ozone loss in the Antarctic and 40 DU in the Arctic. A new finding of this paper is the use of the temporal behavior and variability of ClONO2 and HCl as indicators of the efficacy of heterogeneous chemistry. Transport of ClONO2 from the southern subpolar regions near 55–65°S to higher latitudes near 65–75°S provides a flux of NOx from more sunlit latitudes to the edge of the vortex and is important for ozone loss in this model. Comparisons between modeled and observed total column and profile ozone perturbations, ClONO2 abundances, and the rate of change of HCl bolster confidence in these conclusions.

[1]  Paul J. Crutzen,et al.  Stratospheric aerosol growth and HNO3 gas phase depletion from coupled HNO3 and water uptake by liquid particles , 1994 .

[2]  B. Johnson,et al.  Changes in the Character of Polar Stratospheric Clouds Over Antarctica in 1992 Due to the Pinatubo Volcanic Aerosol , 1994 .

[3]  Daniel R. Marsh,et al.  Climate change from 1850 to 2005 simulated in CESM1(WACCM) , 2013 .

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

[5]  P. Bernath,et al.  Uncertainties in modelling heterogeneous chemistry and Arctic ozone depletion in the winter 2009/2010 , 2012 .

[6]  T. Peter,et al.  Chapter 4:Polar Stratospheric Clouds and Sulfate Aerosol Particles: Microphysics, Denitrification and Heterogeneous Chemistry , 2011 .

[7]  J. Pommereau,et al.  Major influence of tropical volcanic eruptions on the stratospheric aerosol layer during the last decade , 2011 .

[8]  C. B. Farmer,et al.  Infrared aircraft measurements of stratospheric composition over Antarctica during September 1987 , 1989 .

[9]  R. Müller,et al.  Temperature thresholds for chlorine activation and ozone loss in the polar stratosphere , 2012 .

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

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

[12]  D. Worsnop,et al.  Kinetic model for reaction of ClONO2 with H2O and HCl and HOCl with HCl in sulfuric acid solutions , 2001 .

[13]  Roland Neuber,et al.  Nonequilibrium coexistence of solid and liquid particles in Arctic stratospheric clouds , 2001 .

[14]  G. Mann,et al.  The wintertime two-day wave in the polar stratosphere , mesosphere and lower thermosphere , 2008 .

[15]  Larry W. Thomason,et al.  An assessment of CALIOP polar stratospheric cloud composition classification , 2012 .

[16]  Martin Wirth,et al.  Aircraft lidar observations of an enhanced type Ia polar stratospheric clouds during APE‐POLECAT , 1999 .

[17]  Martyn P. Chipperfield,et al.  Arctic ozone loss and climate change , 2004 .

[18]  J. Lamarque,et al.  CAM-chem: description and evaluation of interactive atmospheric chemistry in the Community Earth System Model , 2012 .

[19]  P. Crutzen,et al.  Do stratospheric aerosol droplets freeze above the ice frost point , 1995 .

[20]  Roland Neuber,et al.  Temperature histories in liquid and solid polar stratospheric cloud formation , 1997 .

[21]  P. J. Rasch,et al.  CAM-chem: description and evaluation of interactive atmospheric chemistry in CESM , 2011 .

[22]  P. S. Zurer Arctic Ozone Loss: Fact-Finding Mission Concludes Outlook Is Bleak , 1989 .

[23]  Lamont R. Poole,et al.  Heterogeneous formation of polar stratospheric clouds - Part 1: Nucleation of nitric acid trihydrate (NAT) , 2013 .

[24]  M. Chipperfield,et al.  Modeling the effect of denitrification on Arctic ozone depletion during winter 1999/2000 , 2002 .

[25]  R. Neale,et al.  The Mean Climate of the Community Atmosphere Model (CAM4) in Forced SST and Fully Coupled Experiments , 2013 .

[26]  S. Tilmes,et al.  Chemical and dynamical discontinuity at the extratropical tropopause based on START08 and WACCM analyses , 2011 .

[27]  M. Pitts,et al.  CALIPSO polar stratospheric cloud observations: second-generation detection algorithm and composition discrimination , 2009 .

[28]  Veronika Eyring,et al.  SPARC Report on the Evaluation of Chemistry-Climate Models , 2010 .

[29]  Paul J. Crutzen,et al.  Increase in the PSC‐formation probability caused by high‐flying aircraft , 1991 .

[30]  T. Diehl,et al.  Sensitivity of chemical tracers to meteorological parameters in the MOZART-3 chemical transport model , 2007 .

[31]  L. Froidevaux,et al.  Record-breaking ozone loss in the Arctic winter 2010/2011: comparison with 1996/1997 , 2012 .

[32]  S. Tilmes,et al.  Evaluation of Whole Atmosphere Community Climate Model simulations of ozone during Arctic winter 2004–2005 , 2013 .

[33]  D. R. Hanson,et al.  Heterogeneous reactions in sulfuric acid aerosols: A framework for model calculations , 1994 .

[34]  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 .

[35]  T. Peter,et al.  Ozone depletion in the late winter lower Arctic stratosphere , 1997 .

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

[37]  P. Crutzen,et al.  Size-dependent stratospheric droplet composition in Lee wave temperature fluctuations and their potential role in PSC freezing , 1995 .

[38]  S. Solomon,et al.  Simulation of polar stratospheric clouds in the specified dynamics version of the whole atmosphere community climate model , 2013 .

[39]  D. R. Hanson Reactivity of BrONO2 and HOBr on sulfuric acid solutions at low temperatures , 2003 .

[40]  P. Gent,et al.  Historical Antarctic mean sea ice area, sea ice trends, and winds in CMIP5 simulations , 2013 .

[41]  M. Chipperfield,et al.  A 3D transport model study of chlorine activation during EASOE , 1994 .

[42]  R. Müller,et al.  Uncertainties in reactive uptake coefficients for solid stratospheric particles—2. Effect on ozone depletion , 1997 .

[43]  Stanley C. Solomon,et al.  Stratospheric ozone depletion: A review of concepts and history , 1999 .

[44]  Mark R. Schoeberl,et al.  Unprecedented Arctic ozone loss in 2011 , 2011, Nature.

[45]  R. Turco,et al.  A study of type I polar stratospheric cloud formation , 1994 .

[46]  M. Tesche,et al.  Key Points: @bullet Assessment of Psc Classification Schemes @bullet Statistical Analysis of Psc Observations @bullet Recommendations for Lidar-based Psc Studies Assessing Lidar-based Classification Schemes for Polar Stratospheric Clouds Based on 16 Years of Measurements at Esrange, Sweden , 2022 .

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

[48]  B. Santer,et al.  Influences of the Antarctic Ozone Hole on Southern Hemispheric Summer Climate Change , 2014 .

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

[50]  J. Lelieveld,et al.  Model study of stratospheric chlorine activation and ozone loss during the 1996/1997 winter , 2000 .

[51]  R. Turco,et al.  Condensation of HNO3 and HCl in the winter polar stratospheres , 1986 .

[52]  T. Clarmann,et al.  Arctic winter 2010/2011 at the brink of an ozone hole , 2011 .

[53]  Mark Z. Jacobson,et al.  A model for studying the composition and chemical effects of stratospheric aerosols , 1994 .

[54]  V. L. Orkin,et al.  Chemical Kinetics and Photochemical Data for Use in Atmospheric Studies: Evaluation Number 18 , 2015 .

[55]  D. R. Hanson,et al.  Differences in the reactivity of type I polar stratospheric clouds depending on their phase , 1996 .

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

[57]  Makiko Sato,et al.  Total volcanic stratospheric aerosol optical depths and implications for global climate change , 2014 .

[58]  J. Sheng,et al.  Modeling the stratospheric warming following the Mt. Pinatubo eruption: uncertainties in aerosol extinctions , 2013 .

[59]  E. Castelli,et al.  Extreme ozone depletion in the 2010–2011 Arctic winter stratosphere as observed by MIPAS/ENVISAT using a 2-D tomographic approach , 2012 .

[60]  T. Peter,et al.  Uncertainties in reactive uptake coefficients for solid stratospheric particles‐1. Surface chemistry , 1997 .

[61]  R. Cohen,et al.  Evolution and stoichiometry of heterogeneous processing in the Antarctic stratosphere , 1997 .

[62]  S. Schubert,et al.  MERRA: NASA’s Modern-Era Retrospective Analysis for Research and Applications , 2011 .