scholarly journals Impact of mixing and chemical change on ozone-tracer relations in the polar vortex

2005 ◽  
Vol 5 (4) ◽  
pp. 5841-5874 ◽  
Author(s):  
R. Müller ◽  
S. Tilmes ◽  
P. Konopka ◽  
J.-U. Grooß ◽  
H.-J. Jost
Keyword(s):  
Chemical Change ◽  
Three Dimensional ◽  
Polar Vortex ◽  
Transport Processes ◽  
Lagrangian Model ◽  
Substantial Impact ◽  
Ozone Loss ◽  
Internal Mixing ◽  
Physico Chemical ◽  
Long Time

Abstract. Tracer-tracer relations have been used for a long time to separate physico-chemical change from change caused by transport processes. In particular, for more than a decade, ozone-tracer relations have been used to quantify chemical ozone loss in the polar vortex. The application of ozone-tracer relations for quantifying ozone loss relies on two hypotheses; that a compact ozone-tracer relation is established in the 'early' polar vortex and that any change of the ozone-tracer relation in the vortex over the course of winter is caused predominantly by chemical ozone loss. Here, we revisit this issue analysing various sets of measurements and the results from several models. We find that mixing across the polar vortex edge impacts ozone-tracer relations in a way that may solely lead to an ''underestimation'' of chemical ozone loss and not to an overestimation. Further, differential descent in the vortex and internal mixing has only a negligible impact on ozone loss estimates. Moreover, the representation of mixing in three-dimensional atmospheric models can have a substantial impact on the development of tracer relations in the model. Rather compact ozone-tracer relations develop – in agreement with observations – in the vortex of a Lagrangian model (CLaMS) where mixing is anisotropic and driven by the deformation of the flow. We conclude that, if a reliable 'early vortex' reference can be obtained and if vortex measurements are separated from mid-latitude measurements, ozone-tracer relations constitute a reliable tool for the quantitative determination of chemical ozone loss in the polar vortex.

scholarly journals Impact of mixing and chemical change on ozone-tracer relations in the polar vortex

2005 ◽  
Vol 5 (11) ◽  
pp. 3139-3151 ◽  
Author(s):  
R. Müller ◽  
S. Tilmes ◽  
P. Konopka ◽  
J.-U. Grooß ◽  
H.-J. Jost
Keyword(s):  
Chemical Change ◽  
Three Dimensional ◽  
Polar Vortex ◽  
Transport Processes ◽  
Lagrangian Model ◽  
Substantial Impact ◽  
Ozone Loss ◽  
Internal Mixing ◽  
Physico Chemical ◽  
Long Time

Abstract. Tracer-tracer relations have been used for a long time to separate physico-chemical change from change caused by transport processes. In particular, for more than a decade, ozone-tracer relations have been used to quantify chemical ozone loss in the polar vortex. The application of ozone-tracer relations for quantifying ozone loss relies on two hypotheses: that a compact ozone-tracer relation is established in the 'early' polar vortex and that any change of the ozone-tracer relation in the vortex over the course of winter is caused predominantly by chemical ozone loss. Here, we revisit this issue by analysing various sets of measurements and the results from several models. We find that mixing across the polar vortex edge impacts ozone-tracer relations in a way that may solely lead to an 'underestimation' of chemical ozone loss and not to an overestimation. Further, differential descent in the vortex and internal mixing has only a negligible impact on ozone loss estimates. Moreover, the representation of mixing in three-dimensional atmospheric models can have a substantial impact on the development of tracer relations in the model. Rather compact ozone-tracer relations develop – in agreement with observations – in the vortex of a Lagrangian model (CLaMS) where mixing is anisotropic and driven by the deformation of the flow. We conclude that, if a reliable 'early vortex' reference can be obtained and if vortex measurements are separated from mid-latitude measurements, ozone-tracer relations constitute a reliable tool for the quantitative determination of chemical ozone loss in the polar vortex.

scholarly journals Simulation of denitrification and ozone loss for the Arctic winter 2002/2003

2005 ◽  
Vol 5 (6) ◽  
pp. 1437-1448 ◽  
Author(s):  
J.-U. Grooß ◽  
G. Günther ◽  
R. Müller ◽  
P. Konopka ◽  
S. Bausch ◽  
...  
Keyword(s):  
Inorganic Nitrogen ◽  
Potential Temperature ◽  
Three Dimensional ◽  
Lagrangian Model ◽  
The Arctic ◽  
Particle Nucleation ◽  
Ozone Loss ◽  
Dimensional Version ◽  
Total Inorganic Nitrogen ◽  
Catalytic Cycles

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.

scholarly journals The impact of mid-latitude intrusions into the polar vortex on ozone loss estimates

2003 ◽  
Vol 3 (2) ◽  
pp. 395-402 ◽  
Author(s):  
J.-U. Grooß ◽  
R. Müller
Keyword(s):  
Large Scale ◽  
Loss Rate ◽  
Polar Vortex ◽  
Control Measures ◽  
Lagrangian Model ◽  
The Arctic ◽  
Match Method ◽  
Ozone Loss ◽  
The Impact ◽  
Loss Rates

Abstract. Current stratospheric chemical model simulations underestimate substantially the large ozone loss rates that are derived for the Arctic from ozone sondes for January of some years. Until now, no explanation for this discrepancy has been found. Here, we examine the influence of intrusions of mid-latitude air into the polar vortex on these ozone loss estimates. This study focuses on the winter 1991/92, because during this winter the discrepancy between simulated and experimentally derived ozone loss rates is reported to be the largest. Also during the considered period the vortex was disturbed by a strong warming event with large-scale intrusions of mid-latitude air into the polar vortex, which is quite unusual for this time of the year. The study is based on simulations performed with the Chemical Lagrangian Model of the Stratosphere (CLaMS). Two methods for determination the ozone loss are investigated, the so-called vortex average approach and the Match method. The simulations for January 1992 show that the intrusions induce a reduction of vortex average ozone mixing ratio corresponding to a systematic offset of the ozone loss rate of about 12 ppb per day. This should be corrected for in the vortex average method. The simulations further suggest, that these intrusions do not cause a significant bias for the Match method due to effective quality control measures in the Match technique.

A three-dimensional model comparison of PSC processing during the Arctic winters of 1991/1992 and 1992/1993

1994 ◽  
Vol 12 (4) ◽  
pp. 342-354 ◽  
Author(s):  
M. P. Chipperfield
Keyword(s):  
Model Comparison ◽  
Transport Model ◽  
Three Dimensional ◽  
Polar Vortex ◽  
The Arctic ◽  
Three Dimensional Model ◽  
Polar Stratospheric Clouds ◽  
Ozone Loss ◽  
Stratospheric Clouds ◽  
Compare And Contrast

Abstract. A three-dimensional transport model has been used to compare and contrast the extent of processing by polar stratospheric clouds during the northern hemisphere winters of 1991/1992 and 1992/1993. The model has also been used to compare the potential for ozone loss between these two winters. The TOMCAT off-line model is forced using meteorological analyses from the ECMWF. During winter 1992/1993 polar stratospheric clouds (PSCs) in the model persisted into late February/early March, which is much later than in 1991/1992. This persistence of PSCs should have resulted in much more ozone loss in the later winter. Interestingly, however, the extent of PSC processing and ozone loss was greater in January 1992 than January 1993. In January 1992 PSCs occurred at the edge of a distorted polar vortex whilst in January 1993 the PSCs were located at the centre of a much more zonally symmetrical vortex. In March 1993, distortions of the vortex led to the tearing off of vortex air and its mixing into midlatitudes.

scholarly journals Impact of Lagrangian transport on lower-stratospheric transport timescales in a climate model

2020 ◽  
Vol 20 (23) ◽  
pp. 15227-15245
Author(s):  
Edward J. Charlesworth ◽  
Ann-Kristin Dugstad ◽  
Frauke Fritsch ◽  
Patrick Jöckel ◽  
Felix Plöger
Keyword(s):  
Atmospheric Chemistry ◽  
Large Scale ◽  
Climate Model ◽  
Polar Vortex ◽  
Transport Processes ◽  
Lagrangian Model ◽  
Trace Gas ◽  
Lagrangian Transport ◽  
Transport Barriers ◽  
The Impact

Abstract. We investigate the impact of model trace gas transport schemes on the representation of transport processes in the upper troposphere and lower stratosphere. Towards this end, the Chemical Lagrangian Model of the Stratosphere (CLaMS) was coupled to the ECHAM/MESSy Atmospheric Chemistry (EMAC) model and results from the two transport schemes (Lagrangian critical Lyapunov scheme and flux-form semi-Lagrangian, respectively) were compared. Advection in CLaMS was driven by the EMAC simulation winds, and thereby the only differences in transport between the two sets of results were caused by differences in the transport schemes. To analyze the timescales of large-scale transport, multiple tropical-surface-emitted tracer pulses were performed to calculate age of air spectra, while smaller-scale transport was analyzed via idealized, radioactively decaying tracers emitted in smaller regions (nine grid cells) within the stratosphere. The results show that stratospheric transport barriers are significantly stronger for Lagrangian EMAC-CLaMS transport due to reduced numerical diffusion. In particular, stronger tracer gradients emerge around the polar vortex, at the subtropical jets, and at the edge of the tropical pipe. Inside the polar vortex, the more diffusive EMAC flux-form semi-Lagrangian transport scheme results in a substantially higher amount of air with ages from 0 to 2 years (up to a factor of 5 higher). In the lowermost stratosphere, mean age of air is much smaller in EMAC, owing to stronger diffusive cross-tropopause transport. Conversely, EMAC-CLaMS shows a summertime lowermost stratosphere age inversion – a layer of older air residing below younger air (an “eave”). This pattern is caused by strong poleward transport above the subtropical jet and is entirely blurred by diffusive cross-tropopause transport in EMAC. Potential consequences from the choice of the transport scheme on chemistry–climate and geoengineering simulations are discussed.

scholarly journals The impact of mid-latitude intrusions into the polar vortex on ozone loss estimates

2002 ◽  
Vol 2 (6) ◽  
pp. 2489-2506
Author(s):  
J.-U. Grooß ◽  
R. Müller
Keyword(s):  
Loss Rate ◽  
Polar Vortex ◽  
Lagrangian Model ◽  
The Arctic ◽  
Mixing Ratio ◽  
Match Method ◽  
Air Masses ◽  
Model Simulations ◽  
Ozone Loss ◽  
The Impact

Abstract. Current stratospheric chemical model simulations underestimate substantially the large ozone loss rates that are derived for the Arctic from ozone sondes for January of some years. Until now, no explanation for this discrepancy has been found. Here, we examine the influence of intrusions of mid-latitude air into the polar vortex on these ozone loss estimates. This study focuses on the winter 1991/92. It is based on simulations performed with the Chemical Lagrangian Model of the Stratosphere (CLaMS). The simulations for January 1992 show that the intrusions induce a reduction of vortex average ozone mixing ratio corresponding to a systematic offset of the ozone loss rate of about 12 ppb per day. Further, the results of the Match method are influenced by the intrusions, since the intruded air masses are deformed and reach dimensions below the Match radius. From our calculations we deduce a systematic offset of the Match ozone loss rate by about 10 ppb/day, which may explain about 28% of the published discrepancy between Match and box model simulations for the winter 1991/92.

scholarly journals Mixing and Chemical Ozone Loss during and after the Antarctic Polar Vortex Major Warming in September 2002

2005 ◽  
Vol 62 (3) ◽  
pp. 848-859 ◽  
Author(s):  
Paul Konopka ◽  
Jens-Uwe Grooß ◽  
Karl W. Hoppel ◽  
Hildegard-Maria Steinhorst ◽  
Rolf Müller
Keyword(s):  
Potential Temperature ◽  
Polar Vortex ◽  
Vertical Shear ◽  
Lagrangian Model ◽  
Ozone Loss ◽  
Time Period ◽  
The Difference ◽  
Antarctic Polar Vortex ◽  
The Antarctic ◽  
Vortex Split

Abstract The 3D version of the Chemical Lagrangian Model of the Stratosphere (CLAMS) is used to study the transport of CH4 and O3 in the Antarctic stratosphere between 1 September and 30 November 2002, that is, over the time period when unprecedented major stratospheric warming in late September split the polar vortex into two parts. The isentropic and cross-isentropic velocities in CLAMS are derived from ECMWF winds and heating/cooling rates calculated with a radiation module. The irreversible part of transport, that is, mixing, is driven by the local horizontal strain and vertical shear rates with mixing parameters deduced from in situ observations. The CH4 distribution after the vortex split shows a completely different behavior above and below 600 K. Above this potential temperature level, until the beginning of November, a significant part of vortex air is transported into the midlatitudes up to 40°S. The lifetime of the vortex remnants formed after the vortex split decreases with the altitude with values of about 3 and 6 weeks at 900 and 700 K, respectively. Despite this enormous dynamical disturbance of the vortex, the intact part between 400 and 600 K that “survived” the major warming was strongly isolated from the extravortex air until the end of November. According to CLAMS simulations, the air masses within this part of the vortex did not experience any significant dilution with the midlatitude air. By transporting ozone in CLAMS as a passive tracer, the chemical ozone loss was estimated from the difference between the observed [Polar Ozone and Aerosol Measurement III (POAM III) and Halogen Occultation Experiment (HALOE)] and simulated ozone profiles. Starting from 1 September, up to 2.0 ppmv O3 around 480 K and about 70 Dobson units between 450 and 550 K were destroyed until the vortex was split. After the major warming, no additional ozone loss can be derived, but in the intact vortex part between 450 and 550 K, the accumulated ozone loss was “frozen in” until the end of November.

scholarly journals The impact of transport across the polar vortex edge on Match ozone loss estimates

2008 ◽  
Vol 8 (3) ◽  
pp. 565-578 ◽  
Author(s):  
J.-U. Grooß ◽  
R. Müller ◽  
P. Konopka ◽  
H.-M. Steinhorst ◽  
A. Engel ◽  
...  
Keyword(s):  
Time Integration ◽  
Polar Vortex ◽  
Lagrangian Model ◽  
Match Method ◽  
Ozone Loss ◽  
Air Sampler ◽  
The Impact ◽  
Loss Rates

Abstract. The Match method for the quantification of polar chemical ozone loss is investigated mainly with respect to the impact of the transport of air masses across the vortex edge. For the winter 2002/03, we show that significant transport across the vortex edge occurred and was simulated by the Chemical Lagrangian Model of the Stratosphere. In-situ observations of inert tracers and ozone from HAGAR on the Geophysica aircraft and balloon-borne sondes, and remote observations from MIPAS on the ENVISAT satellite were reproduced well by CLaMS. The model even reproduced a small vortex remnant that remained a distinct feature until June 2003 and was also observed in-situ by a balloon-borne whole air sampler. We use this CLaMS simulation to quantify the impact of transport across the vortex edge on ozone loss estimates from the Match method. We show that a time integration of the determined vortex average ozone loss rates, as performed in Match, results in a larger ozone loss than the polar vortex average ozone loss in CLaMS. The determination of the Match ozone loss rates is also influenced by the transport of air across the vortex edge. We use the model to investigate how the sampling of the ozone sondes on which Match is based represents the vortex average ozone loss rate. Both the time integration of ozone loss and the determination of ozone loss rates for Match are evaluated using the winter 2002/2003 CLaMS simulation. These impacts can explain the majority of the differences between CLaMS and Match column ozone loss. While the investigated effects somewhat reduce the apparent discrepancy in January ozone loss rates reported earlier, a distinct discrepancy between simulations and Match remains. However, its contribution to the accumulated ozone loss over the winter is not large.

scholarly journals Simulation of denitrification and ozone loss for the Arctic winter 2002/2003

2004 ◽  
Vol 4 (6) ◽  
pp. 8069-8101 ◽  
Author(s):  
J.-U. Grooß ◽  
G. Günther ◽  
R. Müller ◽  
P. Konopka ◽  
S. Bausch ◽  
...  
Keyword(s):  
Inorganic Nitrogen ◽  
Potential Temperature ◽  
Three Dimensional ◽  
Lagrangian Model ◽  
The Arctic ◽  
Particle Nucleation ◽  
Ozone Loss ◽  
Dimensional Version ◽  
Total Inorganic Nitrogen ◽  
Catalytic Cycles

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.

scholarly journals The impact of mixing across the polar vortex edge on Match ozone loss estimates

2007 ◽  
Vol 7 (4) ◽  
pp. 11725-11759 ◽  
Author(s):  
J.-U. Grooß ◽  
R. Müller ◽  
P. Konopka ◽  
H.-M. Steinhorst ◽  
A. Engel ◽  
...  
Keyword(s):  
Time Integration ◽  
Polar Vortex ◽  
Lagrangian Model ◽  
Match Method ◽  
Transport Barrier ◽  
Ozone Loss ◽  
The Impact ◽  
Loss Rates

Abstract. The Match method for quantification of polar chemical ozone loss is investigated mainly with respect to the impact of mixing across the vortex edge onto this estimate. We show for the winter 2002/03 that significant mixing across the vortex edge occurred and was accurately modeled by the Chemical Lagrangian Model of the Stratosphere. Observations of inert tracers and ozone in-situ from HAGAR on the Geophysica aircraft and sondes and also remote from MIPAS on ENVISAT were reproduced well. The model even reproduced a small vortex remnant that was isolated until June 2003 and was observed in-situ by a balloon-borne whole air sampler. We use this CLaMS simulation to quantify the impact of cross vortex edge mixing on the results of the Match method. It is shown that a time integration of the determined vortex average ozone loss rates as performed in Match results in larger ozone loss than the polar vortex average ozone loss in CLaMS. Also, the determination of the Match ozone loss rates can be influenced by mixing. This is especially important below 430 K, where ozone outside the vortex is lower than inside and the vortex boundary is not a strong transport barrier. This effect and further sampling effects cause an offset between vortex average ozone loss rates derived from Match and deduced from CLaMS with an even sampling for the entire vortex. Both, the time-integration of ozone loss and the determination of ozone loss rates for Match are evaluated using the winter 2002/03 CLaMS simulation. These impacts can explain the differences between CLaMS and Match column ozone loss. While the investigated effects somewhat reduce the apparent discrepancy in January ozone loss rates, a discrepancy between simulations and Match remains. However, its contribution to the accumulated ozone loss over the winter is not large.

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