Sensitivity of polar stratospheric ozone loss to uncertainties in chemical reaction kinetics
The impact and significance of uncertainties in model calculations of stratospheric ozone loss resulting from known uncertainty in chemical kinetics parameters is evaluated in trajectory chemistry simulations for the Antarctic and Arctic polar vortices. The uncertainty in modeled ozone loss is deriv...
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2009
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ftleibnizopen:oai:oai.leibnizopen.de:BtpQoYoBbHMkKcxzTwKN 2023-10-09T21:47:05+02:00 Sensitivity of polar stratospheric ozone loss to uncertainties in chemical reaction kinetics Kawa, S.R. Stolarski, R.S. Newman, P.A. Douglass, A.R. Rex, M. Hofmann, D.J. Santee, M.L. Frieler, K. 2009 application/pdf https://oa.tib.eu/renate/handle/123456789/5337 https://doi.org/10.34657/3966 eng eng Göttingen : Copernicus GmbH CC BY 3.0 Unported https://creativecommons.org/licenses/by/3.0/ Atmospheric Chemistry and Physics 9 (2009), 22 atmospheric chemistry atmospheric modeling computer simulation in situ measurement laboratory method microwave limb sounder Monte Carlo analysis numerical model observational method ozone parameterization photolysis polar region quantitative analysis reaction kinetics sensitivity analysis stratosphere uncertainty analysis Antarctica Arctic 550 article Text 2009 ftleibnizopen https://doi.org/10.34657/3966 2023-09-17T23:18:12Z The impact and significance of uncertainties in model calculations of stratospheric ozone loss resulting from known uncertainty in chemical kinetics parameters is evaluated in trajectory chemistry simulations for the Antarctic and Arctic polar vortices. The uncertainty in modeled ozone loss is derived from Monte Carlo scenario simulations varying the kinetic (reaction and photolysis rate) parameters within their estimated uncertainty bounds. Simulations of a typical winter/spring Antarctic vortex scenario and Match scenarios in the Arctic produce large uncertainty in ozone loss rates and integrated seasonal loss. The simulations clearly indicate that the dominant source of model uncertainty in polar ozone loss is uncertainty in the Cl2O 2 photolysis reaction, which arises from uncertainty in laboratory-measured molecular cross sections at atmospherically important wavelengths. This estimated uncertainty in J Cl 2O2 from laboratory measurements seriously hinders our ability to model polar ozone loss within useful quantitative error limits. Atmospheric observations, however, suggest that the Cl2O2 photolysis uncertainty may be less than that derived from the lab data. Comparisons to Match, South Pole ozonesonde, and Aura Microwave Limb Sounder (MLS) data all show that the nominal recommended rate simulations agree with data within uncertainties when the Cl2O2 photolysis error is reduced by a factor of two, in line with previous in situ ClOx measurements. Comparisons to simulations using recent cross sections from Pope et al. (2007) are outside the constrained error bounds in each case. Other reactions producing significant sensitivity in polar ozone loss include BrO + ClO and its branching ratios. These uncertainties challenge our confidence in modeling polar ozone depletion and projecting future changes in response to changing halogen emissions and climate. Further laboratory, theoretical, and possibly atmospheric studies are needed. publishedVersion Article in Journal/Newspaper Antarc* Antarctic Antarctica Arctic South pole South pole LeibnizOpen (The Leibniz Association) Arctic Antarctic The Antarctic South Pole |
institution |
Open Polar |
collection |
LeibnizOpen (The Leibniz Association) |
op_collection_id |
ftleibnizopen |
language |
English |
topic |
atmospheric chemistry atmospheric modeling computer simulation in situ measurement laboratory method microwave limb sounder Monte Carlo analysis numerical model observational method ozone parameterization photolysis polar region quantitative analysis reaction kinetics sensitivity analysis stratosphere uncertainty analysis Antarctica Arctic 550 |
spellingShingle |
atmospheric chemistry atmospheric modeling computer simulation in situ measurement laboratory method microwave limb sounder Monte Carlo analysis numerical model observational method ozone parameterization photolysis polar region quantitative analysis reaction kinetics sensitivity analysis stratosphere uncertainty analysis Antarctica Arctic 550 Kawa, S.R. Stolarski, R.S. Newman, P.A. Douglass, A.R. Rex, M. Hofmann, D.J. Santee, M.L. Frieler, K. Sensitivity of polar stratospheric ozone loss to uncertainties in chemical reaction kinetics |
topic_facet |
atmospheric chemistry atmospheric modeling computer simulation in situ measurement laboratory method microwave limb sounder Monte Carlo analysis numerical model observational method ozone parameterization photolysis polar region quantitative analysis reaction kinetics sensitivity analysis stratosphere uncertainty analysis Antarctica Arctic 550 |
description |
The impact and significance of uncertainties in model calculations of stratospheric ozone loss resulting from known uncertainty in chemical kinetics parameters is evaluated in trajectory chemistry simulations for the Antarctic and Arctic polar vortices. The uncertainty in modeled ozone loss is derived from Monte Carlo scenario simulations varying the kinetic (reaction and photolysis rate) parameters within their estimated uncertainty bounds. Simulations of a typical winter/spring Antarctic vortex scenario and Match scenarios in the Arctic produce large uncertainty in ozone loss rates and integrated seasonal loss. The simulations clearly indicate that the dominant source of model uncertainty in polar ozone loss is uncertainty in the Cl2O 2 photolysis reaction, which arises from uncertainty in laboratory-measured molecular cross sections at atmospherically important wavelengths. This estimated uncertainty in J Cl 2O2 from laboratory measurements seriously hinders our ability to model polar ozone loss within useful quantitative error limits. Atmospheric observations, however, suggest that the Cl2O2 photolysis uncertainty may be less than that derived from the lab data. Comparisons to Match, South Pole ozonesonde, and Aura Microwave Limb Sounder (MLS) data all show that the nominal recommended rate simulations agree with data within uncertainties when the Cl2O2 photolysis error is reduced by a factor of two, in line with previous in situ ClOx measurements. Comparisons to simulations using recent cross sections from Pope et al. (2007) are outside the constrained error bounds in each case. Other reactions producing significant sensitivity in polar ozone loss include BrO + ClO and its branching ratios. These uncertainties challenge our confidence in modeling polar ozone depletion and projecting future changes in response to changing halogen emissions and climate. Further laboratory, theoretical, and possibly atmospheric studies are needed. publishedVersion |
format |
Article in Journal/Newspaper |
author |
Kawa, S.R. Stolarski, R.S. Newman, P.A. Douglass, A.R. Rex, M. Hofmann, D.J. Santee, M.L. Frieler, K. |
author_facet |
Kawa, S.R. Stolarski, R.S. Newman, P.A. Douglass, A.R. Rex, M. Hofmann, D.J. Santee, M.L. Frieler, K. |
author_sort |
Kawa, S.R. |
title |
Sensitivity of polar stratospheric ozone loss to uncertainties in chemical reaction kinetics |
title_short |
Sensitivity of polar stratospheric ozone loss to uncertainties in chemical reaction kinetics |
title_full |
Sensitivity of polar stratospheric ozone loss to uncertainties in chemical reaction kinetics |
title_fullStr |
Sensitivity of polar stratospheric ozone loss to uncertainties in chemical reaction kinetics |
title_full_unstemmed |
Sensitivity of polar stratospheric ozone loss to uncertainties in chemical reaction kinetics |
title_sort |
sensitivity of polar stratospheric ozone loss to uncertainties in chemical reaction kinetics |
publisher |
Göttingen : Copernicus GmbH |
publishDate |
2009 |
url |
https://oa.tib.eu/renate/handle/123456789/5337 https://doi.org/10.34657/3966 |
geographic |
Arctic Antarctic The Antarctic South Pole |
geographic_facet |
Arctic Antarctic The Antarctic South Pole |
genre |
Antarc* Antarctic Antarctica Arctic South pole South pole |
genre_facet |
Antarc* Antarctic Antarctica Arctic South pole South pole |
op_source |
Atmospheric Chemistry and Physics 9 (2009), 22 |
op_rights |
CC BY 3.0 Unported https://creativecommons.org/licenses/by/3.0/ |
op_doi |
https://doi.org/10.34657/3966 |
_version_ |
1779309817549029376 |