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Extreme ozone depletion in the 2010–2011 Arctic winter stratosphere as observed by MIPAS/ENVISAT using a 2-D tomographic approach  [PDF]
E. Arnone,E. Castelli,E. Papandrea,M. Carlotti
Atmospheric Chemistry and Physics (ACP) & Discussions (ACPD) , 2012, DOI: 10.5194/acp-12-9149-2012
Abstract: We present observations of the 2010–2011 Arctic winter stratosphere from the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) onboard ENVISAT. Limb sounding infrared measurements were taken by MIPAS during the Northern polar winter and into the subsequent spring, giving a continuous vertically resolved view of the Arctic dynamics, chemistry and polar stratospheric clouds (PSCs). We adopted a 2-D tomographic retrieval approach to account for the strong horizontal inhomogeneity of the atmosphere present under vortex conditions, self-consistently comparing 2011 to the 2-D analysis of 2003–2010. Unlike most Arctic winters, 2011 was characterized by a strong stratospheric vortex lasting until early April. Lower stratospheric temperatures persistently remained below the threshold for PSC formation, extending the PSC season up to mid-March, resulting in significant chlorine activation leading to ozone destruction. On 3 January 2011, PSCs were detected up to 30.5 ± 0.9 km altitude, representing the highest PSCs ever reported in the Arctic. Through inspection of MIPAS spectra, 83% of PSCs were identified as supercooled ternary solution (STS) or STS mixed with nitric acid trihydrate (NAT), 17% formed mostly by NAT particles, and only two cases by ice. In the lower stratosphere at potential temperature 450 K, vortex average ozone showed a daily depletion rate reaching 100 ppbv day 1. In early April at 18 km altitude, 10% of vortex measurements displayed total depletion of ozone, and vortex average values dropped to 0.6 ppmv. This corresponds to a chemical loss from early winter greater than 80%. Ozone loss was accompanied by activation of ClO, associated depletion of its reservoir ClONO2, and significant denitrification, which further delayed the recovery of ozone in spring. Once the PSC season halted, ClO was reconverted primarily into ClONO2. Compared to MIPAS observed 2003–2010 Arctic average values, the 2010–2011 vortex in late winter had 15 K lower temperatures, 40% lower HNO3 and 50% lower ozone, reaching the largest ozone depletion ever observed in the Arctic. The overall picture of this Arctic winter was remarkably closer to conditions typically found in the Antarctic vortex than ever observed before.
Modelling the effect of denitrification on polar ozone depletion for Arctic winter 2004/2005
W. Feng, M. P. Chipperfield, S. Davies, G. W. Mann, K. S. Carslaw, S. Dhomse, L. Harvey, C. Randall,M. L. Santee
Atmospheric Chemistry and Physics (ACP) & Discussions (ACPD) , 2011,
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 2004/2005. 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 ozone loss for Arctic winter 2004/2005 due to the overestimation of denitrification and stronger chlorine activation than observed. A model run with a coupled 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. Overall, denitrification is responsible for a ~30 % enhancement in O3 depletion compared with simulations without denitrification for Arctic winter 2004/2005, which is slightly larger than the inferred impact of denitrification on Arctic ozone loss for previous winters from different CTMs simulations. The overestimated denitrification from standard SLIMCAT simulation causes ~5–10 % more ozone loss at ~17 km compared with the simulation using the DLAPSE PSC scheme for Arctic winter 2004/2005. The calculated partial column ozone loss from SLIMCAT using the DLAPSE scheme is about 130 DU by mid-March 2005, which compares well with the inferred column ozone loss from ozonesondes and satellite data (127±21 DU).
Uncertainties in modeling heterogeneous chemistry and Arctic ozone depletion in the winter 2009/2010
I. Wohltmann,T. Wegner,R. Müller,R. Lehmann
Atmospheric Chemistry and Physics Discussions , 2012, DOI: 10.5194/acpd-12-26245-2012
Abstract: Stratospheric chemistry and denitrification are simulated for the Arctic winter 2009/2010 with the Lagrangian Chemistry and Transport Model ATLAS. A number of sensitivity runs is used to explore the impact of uncertainties in chlorine activation and denitrification on the model results. In particular, the efficiency of chlorine activation on different types of liquid aerosol versus activation on nitric acid trihydrate clouds is examined. Additionally, the impact of changes in reaction rate coefficients, in the particle number density of polar stratospheric clouds, in supersaturation, temperature or the extent of denitrification is investigated. Results are compared to satellite measurements of MLS and ACE-FTS and to in-situ measurements onboard the Geophysica aircraft during the RECONCILE measurement campaign. It is shown that even large changes in the underlying assumptions have only a small impact on the modeled ozone loss, even though they can cause considerable differences in chemical evolution and denitrification. In addition, it is shown that chlorine activation on liquid aerosols alone is able to explain the observed magnitude and morphology of the mixing ratios of active chlorine, reservoir gases and ozone.
Uncertainties in modelling heterogeneous chemistry and Arctic ozone depletion in the winter 2009/2010
I. Wohltmann, T. Wegner, R. Müller, R. Lehmann, M. Rex, G. L. Manney, M. L. Santee, P. Bernath, O. Sumińska-Ebersoldt, F. Stroh, M. von Hobe, C. M. Volk, E. H sen, F. Ravegnani, A. Ulanovsky,V. Yushkov
Atmospheric Chemistry and Physics (ACP) & Discussions (ACPD) , 2013,
Abstract: Stratospheric chemistry and denitrification are simulated for the Arctic winter 2009/2010 with the Lagrangian Chemistry and Transport Model ATLAS. A number of sensitivity runs is used to explore the impact of uncertainties in chlorine activation and denitrification on the model results. In particular, the efficiency of chlorine activation on different types of liquid aerosol versus activation on nitric acid trihydrate clouds is examined. Additionally, the impact of changes in reaction rate coefficients, in the particle number density of polar stratospheric clouds, in supersaturation, temperature or the extent of denitrification is investigated. Results are compared to satellite measurements of MLS and ACE-FTS and to in-situ measurements onboard the Geophysica aircraft during the RECONCILE measurement campaign. It is shown that even large changes in the underlying assumptions have only a small impact on the modelled ozone loss, even though they can cause considerable differences in chemical evolution of other species and in denitrification. Differences in column ozone between the sensitivity runs stay below 10% at the end of the winter. Chlorine activation on liquid aerosols alone is able to explain the observed magnitude and morphology of the mixing ratios of active chlorine, reservoir gases and ozone. This is even true for binary aerosols (no uptake of HNO3 from the gas-phase allowed in the model). Differences in chlorine activation between sensitivity runs are within 30%. Current estimates of nitric acid trihydrate (NAT) number density and supersaturation imply that, at least for this winter, NAT clouds play a relatively small role compared to liquid clouds in chlorine activation. The change between different reaction rate coefficients for liquid or solid clouds has only a minor impact on ozone loss and chlorine activation in our sensitivity runs.
Stratospheric ozone depletion during the 1995–1996 Arctic winter: 3-D simulations on the potential role of different PSC types  [PDF]
J. Hendricks,F. Baier,G. Günther,B. C. Krüger
Annales Geophysicae (ANGEO) , 2003,
Abstract: The sensitivity of modelled ozone depletion in the winter Arctic stratosphere to different assumptions of prevalent PSC types and PSC formation mechanisms is investigated. Three-dimensional simulations of the winter 1995/96 are performed with the COlogne Model of the Middle Atmosphere (COMMA) by applying different PSC microphysical schemes. Model runs are carried out considering either liquid or solid PSC particles or a combined microphysical scheme. These simulations are then compared to a model run which only takes into account binary sulfate aerosols. The results obtained with the three-dimensional model agree with trajectory-box simulations performed in previous studies. The simulations suggest that conditions appropriate for type Ia PSC existence (T < TNAT ) occur over longer periods and cover larger areas when compared to conditions of potential type Ib PSC existence. Significant differences in chlorine activation and ozone depletion occur between the simulations including only either liquid or solid PSC particles. The largest differences, occurring over large spatial scales and during prolonged time periods, are modelled first, when the stratospheric temperatures stay below TNAT , but above the threshold of effective liquid particle growth and second, in the case of the stratospheric temperatures remaining below this threshold, but not falling below the ice frost point. It can be generally concluded from the present study that differences in PSC microphysical schemes can cause significant fluctuations in ozone depletion modelled for the winter Arctic stratosphere. Key words. Atmospheric composition and structure (aerosols and particles; cloud physics and chemistry; middle atmosphere composition and chemistry)
Influence of transport and mixing in autumn on stratospheric ozone variability over the Arctic in early winter
D. Blessmann,I. Wohltmann,M. Rex
Atmospheric Chemistry and Physics (ACP) & Discussions (ACPD) , 2012, DOI: 10.5194/acp-12-7921-2012
Abstract: Early winter ozone mixing ratios in the Arctic middle stratosphere show an interannual variability of about 10%. We show that ozone variability in early January is caused by dynamical processes during Arctic polar vortex formation in autumn (September to December). Observational data from satellites and ozone sondes are used in conjunction with simulations of the chemistry and transport model ATLAS to examine the relationship between the meridional and vertical origin of air enclosed in the polar vortex and its ozone amount. For this, we use a set of artificial model tracers to deduce the origin of the air masses in the vortex in January in latitude and altitude in September. High vortex mean ozone mixing ratios are correlated with a high fraction of air from low latitudes enclosed in the vortex and a high fraction of air that experienced small net subsidence (in a Lagrangian sense). As a measure for the strength of the Brewer-Dobson circulation and meridional mixing in autumn, we use the Eliassen-Palm flux through the mid-latitude tropopause averaged from September to November. In the lower stratosphere, this quantity correlates well with the origin of air enclosed in the vortex and reasonably well with the ozone amount in early winter.
Chemical ozone losses in Arctic and Antarctic polar winter/spring season derived from SCIAMACHY limb measurements 2002–2009
T. Sonkaew, C. von Savigny, K.-U. Eichmann, M. Weber, A. Rozanov, H. Bovensmann, J. P. Burrows,J.-U. Groo
Atmospheric Chemistry and Physics (ACP) & Discussions (ACPD) , 2013,
Abstract: Stratospheric ozone profiles are retrieved for the period 2002–2009 from SCIAMACHY measurements of limb-scattered solar radiation in the Hartley and Chappuis absorption bands of ozone. This data set is used to determine the chemical ozone losses in both the Arctic and Antarctic polar vortices by averaging the ozone in the vortex at a given potential temperature. The chemical ozone losses at isentropic levels between 450 K and 600 K are derived from the difference between observed ozone abundances and the ozone modelled taking diabatic cooling into account, but no chemical ozone loss. Chemical ozone losses of up to 30–40% between mid-January and the end of March inside the Arctic polar vortex are reported. Strong inter-annual variability of the Arctic ozone loss is observed, with the cold winters 2004/2005 and 2006/2007 showing chemical ozone losses inside the polar vortex at 475 K, where 1.7 ppmv and 1.4 ppmv of ozone were removed, respectively, over the period from 22 January to beginning of April and 0.9 ppmv and 1.2 ppmv, respectively, during February. For the winters of 2007/2008 and 2002/2003, ozone losses of about 0.8 ppmv and 0.4 ppmv, respectively are estimated at the 475 K isentropic level for the period from 22 January to beginning of April. Essentially no ozone losses were diagnosed for the relatively warm winters of 2003/2004 and 2005/2006. The maximum ozone loss in the SCIAMACHY data set was found in 2007 at the 600 K level and amounted to about 2.1 ppmv for the period between 22 January and the end of April. Enhanced losses close to this altitude were found in all investigated Arctic springs, in contrast to Antarctic spring. The inter-annual variability of ozone losses and PSC occurrence rates observed during Arctic spring is consistent with the known QBO effects on the Arctic polar vortex, with exception of the unusual Arctic winter 2008/2009. The maximum total ozone mass loss of about 25 million tons was found in the cold Arctic winter of 2004/2005 inside the polar vortex between the 450 K and 600 K isentropic levels from mid-January until the middle of March. The Antarctic vortex averaged ozone loss as well as the size of the polar vortex do not vary much from year to year. The total ozone mass loss inside the Antarctic polar vortex between the 450 K and 600 K isentropic levels is about 50–60 million tons and the vortex volume for this altitude range varies between about 150 and 300 km3 for the period between mid-August and mid-November of every year studied, except for 2002. In 2002 a mid-winter major stratospheric warming occurred in the second half of September and the ozone mass loss was only about half of the value in the other years. However, inside the polar vortex we find chemical ozone losses at the 475 K isentropic level that are similar to those in all other years studied. At this isentropic level ozone losses of 70–90% between mid-August and mid-November or about 2.5 ppmv are observed every year. At isentropic levels
Simulation of denitrification and ozone loss for the Arctic winter 2002/2003
J.-U. Groo , G. Günther, R. Müller, P. Konopka, S. Bausch, H. Schlager, C. Voigt, C.M. Volk,G. C. Toon
Atmospheric Chemistry and Physics (ACP) & Discussions (ACPD) , 2005,
Abstract: We present simulations with the Chemical Lagrangian Model of the Stratosphere (CLaMS) for the Arctic winter 2002/2003. We integrated a Lagrangian denitrification scheme into the three-dimensional version of CLaMS that calculates the growth and sedimentation of nitric acid trihydrate (NAT) particles along individual particle trajectories. From those, we derive the HNO3 downward flux resulting from different particle nucleation assumptions. The simulation results show a clear vertical redistribution of total inorganic nitrogen ( ), with a maximum vortex average permanent removal of over 5ppb in late December between 500 and 550K and a corresponding increase of of over 2ppb below about 450K. The simulated vertical redistribution of is compared with balloon observations by MkIV and in-situ observations from the high altitude aircraft Geophysica. Assuming a globally uniform NAT particle nucleation rate of 7.8x10-6cm-3h-1 in the model, the observed denitrification is well reproduced. In the investigated winter 2002/2003, the denitrification has only moderate impact (≤14%) on the simulated vortex average ozone loss of about 1.1ppm near the 460K level. At higher altitudes, above 600K potential temperature, the simulations show significant ozone depletion through -catalytic cycles due to the unusual early exposure of vortex air to sunlight. Final Revised Paper (PDF, 5810 KB) Discussion Paper (ACPD) Special Issue Citation: Groo , J.-U., Günther, G., Müller, R., Konopka, P., Bausch, S., Schlager, H., Voigt, C., Volk, C.M., and Toon, G. C.: Simulation of denitrification and ozone loss for the Arctic winter 2002/2003, Atmos. Chem. Phys., 5, 1437-1448, doi:10.5194/acp-5-1437-2005, 2005. Bibtex EndNote Reference Manager XML
Simulation of denitrification and ozone loss for the Arctic winter 2002/2003  [PDF]
J.-U. Groo?,G. Günther,R. Müller,P. Konopka
Atmospheric Chemistry and Physics Discussions , 2004,
Abstract: We present simulations with the Chemical Lagrangian Model of the Stratosphere (CLaMS) for the Arctic winter 2002/2003. We integrated a Lagrangian denitrification scheme into the three-dimensional version of CLaMS that calculates the growth and sedimentation of nitric acid trihydrate (NAT) particles along individual particle trajectories. From those, we derive the HNO3 downward flux resulting from different particle nucleation assumptions. The simulation results show a clear vertical redistribution of total inorganic nitrogen (NOy), with a maximum vortex average permanent NOy removal of over 5 ppb in late December between 500 and 550 K and a corresponding increase of NOy of over 2 ppb below about 450 K. The simulated vertical redistribution of NOy is compared with balloon observations by MkIV and in-situ observations from the high altitude aircraft Geophysica. Assuming a globally uniform NAT particle nucleation rate of 3.4·10 6cm 3h 1 in the model, the observed denitrification is well reproduced. In the investigated winter 2002/2003, the denitrification has only moderate impact (≤10%) on the simulated vortex average ozone loss of about 1.1 ppm near the 460 K level. At higher altitudes, above 600 K potential temperature, the simulations show significant ozone depletion through NOx-catalytic cycles due to the unusual early exposure of vortex air to sunlight.
Extrapolating future Arctic ozone losses  [PDF]
B. M. Knudsen,S. B. Andersen,B. Christiansen,N. Larsen
Atmospheric Chemistry and Physics Discussions , 2004,
Abstract: Future increases in the concentration of greenhouse gases and water vapour are likely to cool the stratosphere further and to increase the amount of polar stratospheric clouds (PSCs). Future Arctic PSC areas have been extrapolated using the highly significant trends in the temperature record from 1958–2001. Using a tight correlation between PSC area and the total vortex ozone depletion and taking the decreasing amounts of ozone depleting substances into account we make empirical estimates of future ozone. The result is that Arctic ozone losses increase until 2010–2020 and only decrease slightly up to 2030. This approach is an alternative method of prediction to that based on the complex coupled chemistry-climate models (CCMs).
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