scholarly journals Simple measures of ozone depletion in the polar stratosphere

2007 ◽  
Vol 7 (4) ◽  
pp. 9829-9866
Author(s):  
R. Müller ◽  
J.-U. Grooß ◽  
C. Lemmen ◽  
D. Heinze ◽  
M. Dameris ◽  
...  

Abstract. We investigate the extent to which commonly considered quantities, based on total column ozone observations and simulations, are applicable as measures of ozone loss in the polar vortices. Such quantities have been used frequently in ozone assessments by the World Meteorological Organization (WMO) and to assess the performance of chemistry-climate models. The most commonly considered quantity is monthly mean column ozone poleward of a latitude of 63° in spring. For the Arctic, these monthly means were found to be insensitive to the exact choice of the latitude threshold, unlike the Antarctic where greater sensitivity was found. Choosing a threshold based on the location of the transport barrier at the vortex boundary instead of geometric latitude led to a roughly similar year-to-year variability of the monthly means, but in particular years deviations of several tens of Dobson units occurred. Moreover, the minimum of daily total ozone minima poleward of a particular latitude, another popular measure, is debatable, insofar as it relies on one single measurement or model grid point. For Arctic conditions, this minimum value occurred often in air outside polar vortex, both in the observations and in a chemistry-climate model. As a result, we recommend that the minimum of daily minima no longer be used when comparing polar ozone loss in observations and models. As a possible alternative, we suggest considering the minimum of daily average total ozone poleward of a particular equivalent latitude (or in the vortex) in spring. This definition both obviates relying on one single data point and reduces the impact of year-to-year variability in the Arctic vortex breakup on ozone loss measures. However, compact relations of such simple measures with meteorological quantities that describe the potential for polar heterogeneous chlorine activation and thus ozone loss were not found. Therefore, we argue that where possible, more sophisticated measures of chemical polar ozone loss that include additional information to disentangle the impact of transport and chemistry on ozone, should be employed.

2008 ◽  
Vol 8 (2) ◽  
pp. 251-264 ◽  
Author(s):  
R. Müller ◽  
J.-U. Grooß ◽  
C. Lemmen ◽  
D. Heinze ◽  
M. Dameris ◽  
...  

Abstract. We investigate the extent to which quantities that are based on total column ozone are applicable as measures of ozone loss in the polar vortices. Such quantities have been used frequently in ozone assessments by the World Meteorological Organization (WMO) and also to assess the performance of chemistry-climate models. The most commonly considered quantities are March and October mean column ozone poleward of geometric latitude 63° and the spring minimum of daily total ozone minima poleward of a given latitude. Particularly in the Arctic, the former measure is affected by vortex variability and vortex break-up in spring. The minimum of daily total ozone minima poleward of a particular latitude is debatable, insofar as it relies on one single measurement or model grid point. We find that, for Arctic conditions, this minimum value often occurs in air outside the polar vortex, both in the observations and in a chemistry-climate model. Neither of the two measures shows a good correlation with chemical ozone loss in the vortex deduced from observations. We recommend that the minimum of daily minima should no longer be used when comparing polar ozone loss in observations and models. As an alternative to the March and October mean column polar ozone we suggest considering the minimum of daily average total ozone poleward of 63° equivalent latitude in spring (except for winters with an early vortex break-up). Such a definition both obviates relying on one single data point and reduces the impact of year-to-year variability in the Arctic vortex break-up on ozone loss measures. Further, this measure shows a reasonable correlation (r=–0.75) with observed chemical ozone loss. Nonetheless, simple measures of polar ozone loss must be used with caution; if possible, it is preferable to use more sophisticated measures that include additional information to disentangle the impact of transport and chemistry on ozone.


2018 ◽  
Vol 18 (11) ◽  
pp. 8409-8438 ◽  
Author(s):  
Sandip S. Dhomse ◽  
Douglas Kinnison ◽  
Martyn P. Chipperfield ◽  
Ross J. Salawitch ◽  
Irene Cionni ◽  
...  

Abstract. >We analyse simulations performed for the Chemistry-Climate Model Initiative (CCMI) to estimate the return dates of the stratospheric ozone layer from depletion caused by anthropogenic stratospheric chlorine and bromine. We consider a total of 155 simulations from 20 models, including a range of sensitivity studies which examine the impact of climate change on ozone recovery. For the control simulations (unconstrained by nudging towards analysed meteorology) there is a large spread (±20 DU in the global average) in the predictions of the absolute ozone column. Therefore, the model results need to be adjusted for biases against historical data. Also, the interannual variability in the model results need to be smoothed in order to provide a reasonably narrow estimate of the range of ozone return dates. Consistent with previous studies, but here for a Representative Concentration Pathway (RCP) of 6.0, these new CCMI simulations project that global total column ozone will return to 1980 values in 2049 (with a 1σ uncertainty of 2043–2055). At Southern Hemisphere mid-latitudes column ozone is projected to return to 1980 values in 2045 (2039–2050), and at Northern Hemisphere mid-latitudes in 2032 (2020–2044). In the polar regions, the return dates are 2060 (2055–2066) in the Antarctic in October and 2034 (2025–2043) in the Arctic in March. The earlier return dates in the Northern Hemisphere reflect the larger sensitivity to dynamical changes. Our estimates of return dates are later than those presented in the 2014 Ozone Assessment by approximately 5–17 years, depending on the region, with the previous best estimates often falling outside of our uncertainty range. In the tropics only around half the models predict a return of ozone to 1980 values, around 2040, while the other half do not reach the 1980 value. All models show a negative trend in tropical total column ozone towards the end of the 21st century. The CCMI models generally agree in their simulation of the time evolution of stratospheric chlorine and bromine, which are the main drivers of ozone loss and recovery. However, there are a few outliers which show that the multi-model mean results for ozone recovery are not as tightly constrained as possible. Throughout the stratosphere the spread of ozone return dates to 1980 values between models tends to correlate with the spread of the return of inorganic chlorine to 1980 values. In the upper stratosphere, greenhouse gas-induced cooling speeds up the return by about 10–20 years. In the lower stratosphere, and for the column, there is a more direct link in the timing of the return dates of ozone and chlorine, especially for the large Antarctic depletion. Comparisons of total column ozone between the models is affected by different predictions of the evolution of tropospheric ozone within the same scenario, presumably due to differing treatment of tropospheric chemistry. Therefore, for many scenarios, clear conclusions can only be drawn for stratospheric ozone columns rather than the total column. As noted by previous studies, the timing of ozone recovery is affected by the evolution of N2O and CH4. However, quantifying the effect in the simulations analysed here is limited by the few realisations available for these experiments compared to internal model variability. The large increase in N2O given in RCP 6.0 extends the ozone return globally by ∼ 15 years relative to N2O fixed at 1960 abundances, mainly because it allows tropical column ozone to be depleted. The effect in extratropical latitudes is much smaller. The large increase in CH4 given in the RCP 8.5 scenario compared to RCP 6.0 also lengthens ozone return by ∼ 15 years, again mainly through its impact in the tropics. Overall, our estimates of ozone return dates are uncertain due to both uncertainties in future scenarios, in particular those of greenhouse gases, and uncertainties in models. The scenario uncertainty is small in the short term but increases with time, and becomes large by the end of the century. There are still some model–model differences related to well-known processes which affect ozone recovery. Efforts need to continue to ensure that models used for assessment purposes accurately represent stratospheric chemistry and the prescribed scenarios of ozone-depleting substances, and only those models are used to calculate return dates. For future assessments of single forcing or combined effects of CO2, CH4, and N2O on the stratospheric column ozone return dates, this work suggests that it is more important to have multi-member (at least three) ensembles for each scenario from every established participating model, rather than a large number of individual models.


2018 ◽  
Author(s):  
Sandip Dhomse ◽  
Douglas Kinnison ◽  
Martyn P. Chipperfield ◽  
Irene Cionni ◽  
Michaela Hegglin ◽  
...  

Abstract. We analyse simulations performed for the Chemistry-Climate Model Initiative (CCMI) to estimate the return dates of the stratospheric ozone layer from depletion caused by anthropogenic stratospheric chlorine and bromine. We consider a total of 155 simulations from 20 models, including a range of sensitivity studies which examine the impact of climate change on ozone recovery. For the control simulations (unconstrained by nudging towards analysed meteorology) there is a large spread (±20 DU in the global average) in the predictions of the absolute ozone column. Therefore, the model results need to be adjusted for biases against historical data. Also, the interannual variability in the model results need to be smoothed in order to provide a reasonably narrow estimate of the range of ozone return dates. Consistent with previous studies, but here for a Representative Concentration Pathway (RCP) of 6.0, these new CCMI simulations project that global total column ozone will return to 1980 values in 2047 (with a 1-σ uncertainty of 2042–2052). At Southern Hemisphere mid-latitudes column ozone is projected to return to 1980 values in 2046 (2042–2050), and at Northern Hemisphere mid-latitudes in 2034 (2024–2044). In the polar regions, the return dates are 2062 (2055–2066) in the Antarctic in October and 2035 (2025–2040) in the Arctic in March. The earlier return dates in the NH reflect the larger sensitivity to dynamical changes. Our estimates of return dates are later than those presented in the 2014 Ozone Assessment by approximately 5–15 years, depending on the region. In the tropics only around half the models predict a return to 1980 values, at around 2040, while the other half do not reach this value. All models show a negative trend in tropical total column ozone towards the end of the 21st century. The CCMI models generally agree in their simulation of the time evolution of stratospheric chlorine, which is the main driver of ozone loss and recovery. However, there are a few outliers which show that the multi-model mean results for ozone recovery are not as tightly constrained as possible. Throughout the stratosphere the spread of ozone return dates to 1980 values between models tends to correlate with the spread of the return of inorganic chlorine to 1980 values. In the upper stratosphere, greenhouse gas-induced cooling speeds up the return by about 10–20 years. In the lower stratosphere, and for the column, there is a more direct link in the timing of the return dates, especially for the large Antarctic depletion. Comparisons of total column ozone between the models is affected by different predictions of the evolution of tropospheric ozone within the same scenario, presumably due to differing treatment of tropospheric chemistry. Therefore, for many scenarios, clear conclusions can only be drawn for stratospheric ozone columns rather than the total column. As noted by previous studies, the timing of ozone recovery is affected by the evolution of N2O and CH4. However, the effect in the simulations analysed here is small and at the limit of detectability from the few realisations available for these experiments compared to internal model variability. The large increase in N2O given in RCP 6.0 extends the ozone return globally by ~ 15 years relative to N2O fixed at 1960 abundances, mainly because it allows tropical column ozone to be depleted. The effect in extratropical latitudes is much smaller. The large increase in CH4 given in the RCP 8.5 scenario compared to RCP 6.0 also changes ozone return by ~ 15 years, again mainly through its impact in the tropics. For future assessments of single forcing or combined effects of CO2, CH4, and N2O on the stratospheric column ozone return dates, this work suggests that is more important to have multi-member (at least 3) ensembles for each scenario from each established participating model, rather than a large number of individual models.


2011 ◽  
Vol 11 (2) ◽  
pp. 3857-3884 ◽  
Author(s):  
W. Feng ◽  
M. P. Chipperfield ◽  
S. Davies ◽  
G. W. Mann ◽  
K. S. Carslaw ◽  
...  

Abstract. A three-dimensional (3-D) chemical transport model (CTM), SLIMCAT, has been used to quantify the effect of denitrification on ozone loss for the Arctic winter/spring 2004/05. The simulated HNO3 is found to be highly sensitive to the polar stratospheric cloud (PSC) scheme used in the model. Here the standard SLIMCAT full chemistry model, which uses a thermodynamic equilibrium PSC scheme, overpredicts the Arctic ozone loss for Arctic winter/spring 2004/05 due to the overestimation of denitrification and stronger chlorine activation than observed. A model run with a detailed microphysical denitrification scheme, DLAPSE (Denitrification by Lagrangian Particle Sedimentation), is less denitrified than the standard model run and better reproduces the observed HNO3 as measured by Airborne SUbmillimeter Radiometer (ASUR) and Aura Microwave Limb Sounder (MLS) instruments. The overestimated denitrification causes a small overestimation of Arctic polar ozone loss (~5–10% at ~17 km) by the standard model. Use of the DLAPSE scheme improves the simulation of Arctic ozone depletion compared with the inferred partial column ozone loss from ozonesondes and satellite data. Overall, denitrification is responsible for a ~30% enhancement in O3 depletion for Arctic winter/spring 2004/05, suggesting that the successful simulation of the impact of denitrification on Arctic ozone depletion also requires the use of a detailed microphysical PSC scheme in the model.


2018 ◽  
Author(s):  
Xiaoyi Zhao ◽  
Kristof Bognar ◽  
Vitali Fioletov ◽  
Andrea Pazmino ◽  
Florence Goutail ◽  
...  

Abstract. Zenith-Sky scattered light Differential Optical Absorption Spectroscopy (ZS-DOAS) has been used widely to retrieve total column ozone (TCO). ZS-DOAS measurements have the advantage of being less sensitive to clouds than direct-sun measurements. However, the presence of clouds still affects the quality of ZS-DOAS TCO. Clouds are thought to be the largest contributor to random uncertainty in ZS-DOAS TCO, but their impact on data quality still needs to be quantified. This study has two goals: (1) to study whether clouds have a significant impact on ZS-DOAS TCO, and (2) to develop a cloud-screening algorithm to improve ZS-DOAS measurements in the Arctic under cloudy conditions. To quantify the impact of weather, eight years of measured and modelled TCO have been used, along with information about weather conditions at Eureka, Canada (80.05° N, 86.41° W). Relative to direct-sun TCO measurements by Brewer spectrophotometers and modelled TCO, a positive bias is found in ZS-DOAS TCO measured in cloudy weather, and a negative bias is found for clear conditions, with differences of up to 5 % between clear and cloudy conditions. A cloud-screening algorithm is developed for high-latitudes using the colour index calculated from ZS-DOAS spectra. The quality of ZS-DOAS TCO datasets is assessed using a statistical uncertainty estimation model, which suggests a 3–4 % random uncertainty. The new cloud-screening algorithm reduces the random uncertainty by 0.6 %. If all measurements collected during cloudy conditions, as identified using the weather station observations, are removed, the random uncertainty is reduced by 1.3 %. This work demonstrates that clouds are a significant contributor to uncertainty in ZS-DOAS TCO and proposes a method that can be used to screen clouds in high-latitude spectra.


2004 ◽  
Vol 4 (5) ◽  
pp. 5019-5044
Author(s):  
F. Goutail ◽  
J.-P. Pommereau ◽  
F. Lefèvre ◽  
M. Van Roozendael ◽  
S. B. Andersen ◽  
...  

Abstract. Total column ozone reduction in the Arctic is evaluated each winter since 1993/1994 by the transport method (3-D CTM passive ozone minus measurements). The cumulative loss from 1 December to the end of the season ranges from 5–10% during warm winters like 1998/1999, 2000/2001 and 2001/2002 up to 30%–32% during cold winters like 1994/1995 and 1995/1996. The 23% cumulative loss observed during the winter 2002/2003 is similar in amplitude to the 20–24% measured in 1996/1997 and 1999/2000 but the timing is different. It started unusually early in December after the occurrence of very low temperature at all stratospheric levels between 550 K and 435 K allowing PSC formation and thus chlorine activation. The early ozone loss of 2002/2003 is well captured by current 3-D CTM models.


2009 ◽  
Vol 9 (22) ◽  
pp. 8651-8660 ◽  
Author(s):  
S. R. Kawa ◽  
R. S. Stolarski ◽  
P. A. Newman ◽  
A. R. Douglass ◽  
M. Rex ◽  
...  

Abstract. 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 Cl2O2 photolysis reaction, which arises from uncertainty in laboratory-measured molecular cross sections at atmospherically important wavelengths. This estimated uncertainty in JCl2O2 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.


2019 ◽  
Vol 19 (1) ◽  
pp. 577-601 ◽  
Author(s):  
Debora Griffin ◽  
Kaley A. Walker ◽  
Ingo Wohltmann ◽  
Sandip S. Dhomse ◽  
Markus Rex ◽  
...  

Abstract. Stratospheric ozone loss inside the Arctic polar vortex for the winters between 2004–2005 and 2012–2013 has been quantified using measurements from the space-borne Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS). For the first time, an evaluation has been performed of six different ozone loss estimation methods based on the same single observational dataset to determine the Arctic ozone loss (mixing ratio loss profiles and the partial-column ozone losses between 380 and 550 K). The methods used are the tracer-tracer correlation, the artificial tracer correlation, the average vortex profile descent, and the passive subtraction with model output from both Lagrangian and Eulerian chemical transport models (CTMs). For the tracer-tracer, the artificial tracer, and the average vortex profile descent approaches, various tracers have been used that are also measured by ACE-FTS. From these seven tracers investigated (CH4, N2O, HF, OCS, CFC-11, CFC-12, and CFC-113), we found that CH4, N2O, HF, and CFC-12 are the most suitable tracers for investigating polar stratospheric ozone depletion with ACE-FTS v3.5. The ozone loss estimates (in terms of the mixing ratio as well as total column ozone) are generally in good agreement between the different methods and among the different tracers. However, using the average vortex profile descent technique typically leads to smaller maximum losses (by approximately 15–30 DU) compared to all other methods. The passive subtraction method using output from CTMs generally results in slightly larger losses compared to the techniques that use ACE-FTS measurements only. The ozone loss computed, using both measurements and models, shows the greatest loss during the 2010–2011 Arctic winter. For that year, our results show that maximum ozone loss (2.1–2.7 ppmv) occurred at 460 K. The estimated partial-column ozone loss inside the polar vortex (between 380 and 550 K) using the different methods is 66–103, 61–95, 59–96, 41–89, and 85–122 DU for March 2005, 2007, 2008, 2010, and 2011, respectively. Ozone loss is difficult to diagnose for the Arctic winters during 2005–2006, 2008–2009, 2011–2012, and 2012–2013, because strong polar vortex disturbance or major sudden stratospheric warming events significantly perturbed the polar vortex, thereby limiting the number of measurements available for the analysis of ozone loss.


2009 ◽  
Vol 9 (3) ◽  
pp. 13327-13354
Author(s):  
S. R. Kawa ◽  
R. S. Stolarski ◽  
P. A. Newman ◽  
A. R. Douglass ◽  
M. Rex ◽  
...  

Abstract. 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 Cl2O2 photolysis reaction, which arises from uncertainty in laboratory-measured molecular cross sections at atmospherically important wavelengths. This estimated uncertainty in JCl2O2 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.


2018 ◽  
Author(s):  
Debora Griffin ◽  
Kaley A. Walker ◽  
Ingo Wohltmann ◽  
Sandip S. Dhomse ◽  
Markus Rex ◽  
...  

Abstract. Stratospheric ozone loss inside the Arctic polar vortex for the winters between 2004/2005 and 2012/2013 has been quantified using measurements from the space-borne Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS). Six different methods, including tracer-tracer correlation, artificial tracer correlation, average vortex profile descent, and passive subtraction with model output from both Lagrangian and Eulerian chemical transport models (CTMs), have been employed to determine the Arctic ozone loss (mixing ratio loss profiles and the partial column ozone losses between 380 and 550 K). For the tracer-tracer, the artificial tracer, and the average vortex profile descent approaches, various tracers have been used. Here, we show that CH4, N2O, HF, and CFC-12 are suitable tracers for investigating polar stratospheric ozone depletion with ACE-FTS. The ozone loss estimates (in terms of the mixing ratio as well as total column ozone) are generally in good agreement between the different methods and among the different tracers. However, the tracer-tracer correlation method does not agree with the other estimation methods in March 2005 and using the average vortex profile descent technique typically leads to smaller maximum losses compared to all other methods. The passive subtraction method using output from CTMs generally results in smaller uncertainties and slightly larger losses compared to the techniques that use ACE-FTS measurements only. The ozone loss computed, using both measurements and models, shows the greatest loss during the 2010/2011 Arctic winter. For that year, our results show that maximum ozone loss (2.1–2.7 ppmv) occurred at 460 K. The estimated partial column ozone loss inside the polar vortex (between 380 K and 550 K) is 66–103 DU, 61–95 DU, 59–96 DU, 41–89 DU, and 85–122 DU for March 2005, 2007, 2008, 2010, and 2011, respectively. Ozone loss is difficult to diagnose during 2005/2006, 2008/2009, 2011/2012, and 2012/2013 because strong polar vortex disturbance or major sudden stratospheric warming events significantly perturbed the polar vortex thereby limiting the number of measurements available for the analysis.


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