A SPARC Success Story: The Role of Halogen Chemistry in Polar Stratospheric Ozone Depletion

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1 A SPARC Success Story: The Role of Halogen Chemistry in Polar Stratospheric Ozone Depletion An Update on the Initiative Sponsored by the Stratospheric Processes and their Role in Climate (SPARC) Project of the World Climate Research Programme Initiative Co-Chairs: Michael J. Kurylo (UMBC/GEST) Björn-Martin Sinnhuber (U. Bremen) WCRP SPARC Scientific Steering Group 17 th Session Kyoto, Japan October 2009

2 ClOOCl Spectral and Absorption Cross-Section Data Available for the JPL 06-2 Evaluation Cross Section (cm 2 molecule -1 ) Cox and Hayman (1988) Burkholder et al. (1990) DeMore and Tschuikow (1990) Vogt and Schindler (1990) Molina et al. (1990) Huder and DeMore (1995) Bloss et al. (2001) McKeachie et al. (2004) JPL Wavelength (nm)

3 A Greater Problem Arises Cross Section (cm 2 molecule -1 ) Cox and Hayman (1988) Burkholder et al. (1990) DeMore and Tschuikow (1990) Vogt and Schindler (1990) Molina et al. (1990) Huder and DeMore (1995) Bloss et al. (2001) McKeachie et al. (2004) JPL 2006 Pope et al. (2007) Wavelength (nm)

4 Models Using Pope et al. Cross Sections Yield Less O 3 Loss than Observed: Antarctic simulation using CLAMS model Huder & DeMore 1994 JPL 2006 Pope 2007 JPL 2006 Burkholder 1990 Observed Ozone von Hobe et al., ACP, 2007

5 Models Using Pope et al. Cross Sections Yield Less O 3 Loss than Observed: Arctic simulation using box model constrained by observed ClO x Calculated Ozone Loss for Model Constrained by SOLVE Measurements of ClO+2 ClOOCl Modeled Ozone Loss for: GREEN DASHED: Pope et al. (2007), BrO from CH 3 Br & Halons GREEN SOLID : Pope et al. (2007), measured BrO JPL 2006 Observed Ozone Loss, Match Modeled Ozone Loss for: BLACK : JPL 02 Kinetics, BrO from CH 3 Br & Halons BLUE DOTTED : JPL 02 Kinetics, BrOx from measured BrO BLUE DASHED: JPL 02 Kinetics except Burkholder et al. (1990) cross section BLUE SOLID : Burkholder et al. (1990) cross section and measured BrO Figure 4-17, WMO 2007, adapted from Frieler et al., GRL, 2006 Updated to include Pope et al. cross section by R. Schofield, M. Rex, T. Canty and R. Salawitch

6 Pope et al. cross sections in MOZART3/WACCM1b yield half as much ozone loss as Burkholder et al. cross sections 0 pptv Bry 22 pptv Bry Kinnison, Brasseur, Orlando, Garcia, Tilmes

7 The UV/Vis Absorption Spectrum of Matrix-Isolated Dichlorine Peroxide, ClOOCl M. von Hobe, F. Stroh, H. Beckers, T. Benter, and H. Willner Phys. Chem. Chem. Phys., 2009, 11, , DOI: /b814373k ClOOCl Cross Section (cm 2 ) Burkholder et al., 1990 JPL 2006 Huder and DeMore, 1995 von Hobe et al., 2008 Pope et al., 2007

8 More Recent Published Gas Phase Spectra Chen et al., UV Absorption Cross Sections of ClOOCl are Consistent with Ozone Degradation Models, Science, 324, 781, 8 May 2009.

9 NASA / JPL Data Panel Interim Recommendation "Chemical Kinetics and Photochemical Data for Use in Atmospheric Studies Evaluation Number 16 of the NASA Panel for Data Evaluation", JPL Publication 09-XX (2009). S. P. Sander, R. R. Friedl, D. M. Golden, M. J. Kurylo, P. H. Wine, J. Abbatt, J. B. Burkholder, C. E. Kolb, G. K. Moortgat, R. E. Huie, and V. L. Orkin Soon to be available at jpldataeval.jpl.nasa.gov/.

10 NASA / JPL 09: Estimated Error Limits Revised Cross Section (cm 2 molecule -1 ) Wavelength (nm)

11 Chlorine- Catalyzed Ozone Destruction: Cl Atom Production from ClOOCl Photolysis D. M. Wilmouth, T. F. Hanisco, R. M. Stimpfle, and J. G. Anderson J. Phys. Chem. (in press) Available for download on the J. Phys Chem A ASAP website: pdf/ /jp

12 Chlorine-Catalyzed Ozone Destruction: Cl Atom Production from ClOOCl Photolysis Wilmouth et al., J. Phys. Chem. (in press)

13 Chlorine-Catalyzed Ozone Destruction: Cl Atom Production from ClOOCl Photolysis Wilmouth et al., J. Phys. Chem. (in press)

14 UV Absorption Spectrum of the ClO Dimer (Cl2O2) between 200 and 420 nm D. K. Papanastasiou, V. C. Papadimitriou, D. W. Fahey, and J. B. Burkholder J. Phys. Chem. (in press)

15 UV Absorption Spectrum of the ClO Dimer (Cl2O2) between 200 and 420 nm D. K. Papanastasiou, V. C. Papadimitriou, D. W. Fahey, and J. B. Burkholder J. Phys. Chem. (in press) Comparison of wavelength dependent Cl 2 O 2 atmospheric photolysis rate coefficients, J(λ), calculated for a solar zenith angle (SZA) of 86 at an altitude of 20 km

16 UV Absorption Spectrum of the ClO Dimer (Cl2O2) between 200 and 420 nm D. K. Papanastasiou, V. C. Papadimitriou, D. W. Fahey, and J. B. Burkholder J. Phys. Chem. (in press) Upper Frame: Integrated atmospheric photolysis rate coefficients, J, calculated for Cl 2 O 2 as a function of solar zenith angle (SZA). Lower Frame: Same data relative to the values obtained using the NASA/JPL recommended Cl 2 O 2 cross section data.

17 JPL 09 Recommendation & Most Recent Lab Studies Cross Section (cm 2 molecule -1 ) JPL 09 JPL 09 Est. Error IUPAC (2007) Pope et al. (2007) von Hobe et al. (2009) Chen et al. (2009) Wilmouth et al. (2009) Papanastasiou et al. (2009) 2.5 σ / σ(jpl 09) Wavelength (nm)

18 Conclusions The ClOOCl cross section has been perhaps the largest source of uncertainty in our description of polar ozone loss. The laboratory measurement of the ClOOCl cross section by Pope et al. (2007) fell outside the range of uncertainty defined by prior laboratory studies, leading to much discussion, deliberation, and debate within the atmospheric chemistry community. The community met in Cambridge, England (June 2008) to examine our understanding of polar ozone loss (laboratory, theory, field observations, and modelling) in light of the Pope et al. study. A detailed report from that workshop is available electronically at: Several subsequent laboratory studies (published or about to be published) have failed to reproduce the Pope et al. ClOOCl cross sections and provide strong support for our understanding of chlorine-catalyzed ozone loss in the polar stratosphere. The SPARC Initiative played an important role in fostering this new work!

19 JPL-09 Recommendations on the ClO + ClO ClOOCl Equilibrium Constant "Chemical Kinetics and Photochemical Data for Use in Atmospheric Studies Evaluation Number 16 of the NASA Panel for Data Evaluation", JPL Publication 09-XX (2009). S. P. Sander, R. R. Friedl, D. M. Golden, M. J. Kurylo, P. H. Wine, J. Abbatt, J. B. Burkholder, C. E. Kolb, G. K. Moortgat, R. E. Huie, and V. L. Orkin Soon to be available at

20 Lab Data Used in the JPL 2009 Recommendation for K EQ Over the Temperature Range 180<T/K< K = 1.72x10-27 exp(8649/t) K298 = 6.9x ClO = Cl 2 O f(t) = 1.25*exp(200* ((1/298)-(1/T)) [f(t) 2 = 95%] Shown Log K/cm 3 molecule rd Law with the data points from Cox and Nickolaisen and structures and frequencies from Golden with hindered rotor from Barker. JPL 2009 [+95%] [-95%] Nickolaisenet al. Cox Boakes Horowitz Ellerman /T

21 Lab Data Together with Various Fits for K EQ Over the Temperature Range 180<T/K< ClO = Cl 2 O K = 1.72x10-27 exp(8649/t) Log K/cm 3 molecule K298 = 6.9x10-15 f(t) = 1.25*exp(200* ((1/298)-(1/T)) [f(t) 2 = 95%] Shown JPL 2009 [+95%] [-95%] Nickolaisenet al. Cox Plenge 2 parameter Avallone & Toohey von Hobe 2005 Broske Boakes Horowitz Ellerman /T

22 JPL 2006 and JPL 2009 Recommendations for K EQ Together with Various Fits from 180 < T/K < 225 K = 1.72x10-27 exp(8649/t) 2ClO = Cl 2 O 2 Log K/cm 3 molecule K298 = 6.9x10-15 f(t) = 1.25*exp(200* ((1/298)-(1/T)) [f(t) 2 = 95%] Shown 3rd Law with the data points from Cox and Nickolaisen and structures and frequencies from Golden with hindered rotor from Barker /T JPL 2009 JPL 2006 [+95%] [-95%] Plenge 2 parameter Avallone & Toohey von Hobe 2005 May 24, 2009

23 Salawitch / Canty Analysis of Field Data Filtered for SZA > 105 Displayed on the Previous Plot -5.0 K = 1.72x10-27 exp(8649/t) 2ClO =Cl 2 O 2 Log K/cm 3 molecule K298 = 6.9x10-15 f(t) = 1.25*exp(200* ((1/298)-(1/T)) [f(t) 2 = 95%] Shown 180K JPL E-6 A&T 8.32E-7 von Hobe 1.82E-7 JPL 2009 JPL 2006 [+95%] [-95%] Plenge 2 parameter rd Law with the data points from Cox and Nickolaisen and structures and frequencies from Golden with hindered rotor from Barker. Avallone & Toohey von Hobe 2005 Ross sza > /T May 24, 2009

24 Constraining the ClO/ClOOCl Equilibrium Constant from Aura Microwave Limb Sounder Measurements of Nighttime ClO M. Santee, S. Sander, N. Livesey and L. Froidevaux (to be submitted to PNAS Special Issue on Atmospheric Chemistry)

25 Acknowledgements NASA/JPL Panel for Data Evaluation esp. D. Golden & J. Burkholder New Lab Studies D. Wilmouth & J. Anderson (Harvard U.) J. Burkholder (NOAA-ESRL)

26 Interface between Laboratory Kinetics and the 2010 WMO/UNEP Ozone Assessment Lifetimes for Long-Lived Compounds and VSLS s for Chapters 1 and 5 Based on the most current JPL 2010 and IUPAC Evaluations "Chemical Kinetics and Photochemical Data for Use in Atmospheric Studies Evaluation Number 17 of the NASA Panel for Data Evaluation JPL Publication 10-XX (2010). S. P. Sander, R. R. Friedl, D. M. Golden, M. J. Kurylo, P. H. Wine, J. Abbatt, J. B. Burkholder, C. E. Kolb, G. K. Moortgat, R. E. Huie, and V. L. Orkin Available Spring 2010 at

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35 Influence of JPL 09 XX Recommenda5ons on Model Simula5ons of NO y and O 3 Charles Jackman and Eric Fleming September 29, 2009 GSFC Fully Coupled 2 D Model Computa5ons of Cons5tuent Diurnal Cycles 1) Compare with UARS odd nitrogen (NO,NO 2,HNO 3,ClONO 2 ) 2) Compare with Total Ozone Measurements ( ) 3) Total Ozone (1980, 2000, 5me series)

36 1) Compare with UARS odd nitrogen (NO, NO 2, HNO 3, ClONO 2 ) NO+NO 2 at Sunset; HNO 3 +ClONO 2 for 24-hour average Model with JPL-09 higher than with JPL-06 [due to increased N 2 O + O( 1 D) 2NO reaction]

37 2) Compare with Total Ozone Measurements ( ) Total Ozone average Model with JPL-09 lower than with JPL-06 Largest impact in polar spring, especially SH [~One-half of change due to increased N 2 O + O( 1 D) 2NO reaction] -10 DU -15 DU

38 3) Total Ozone (1980, 2000, time series) Model with JPL-09 has less ozone than with JPL-06 (higher Cl sensitivity in polar regions with JPL-09) Ozone recovery delayed by ~1 year

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