scholarly journals Vortex-wide chlorine activation by a mesoscale PSC event in the Arctic winter of 2009/10

2015 ◽  
Vol 15 (22) ◽  
pp. 33731-33754
Author(s):  
T. Wegner ◽  
M. C. Pitts ◽  
L. R. Poole ◽  
I. Tritscher ◽  
J.-U. Grooß ◽  
...  

Abstract. In the Arctic polar vortex of the 2009/10 winter temperatures were low enough to allow widespread formation of Polar Stratospheric Clouds (PSC). These clouds occurred during the initial chlorine activation phase which provided the opportunity to investigate the impact of PSCs on chlorine activation. Satellite observations of gas-phase species and PSCs are used in combination with trajectory modeling to assess this initial activation. The initial activation occurred in association with the formation of PSCs over the east coast of Greenland at the beginning of January 2010. Although this area of PSCs covered only a small portion of the vortex, it was responsible for almost the entire initial activation of chlorine vortex wide. Observations show HCl mixing ratios decreased rapidly in and downstream of this region. Trajectory calculations and simplified heterogeneous chemistry modeling confirmed that the initial chlorine activation continued until ClONO2 was completely depleted and the activated air masses were advected throughout the polar vortex. For the calculation of heterogeneous reaction rates, surface area density is estimated from backscatter observations. Modeled heterogeneous reaction rates along trajectories intersecting with the PSC indicate that the initial phase of chlorine activation occurred in just a few hours. These calculations also indicate that chlorine activation on the binary background aerosol is significantly slower than on the PSCs and the observed chlorine activation can only be explained by an increase in surface area density due to PSCs. Furthermore, there is a strong correlation between the magnitude of the observed HCl depletion and PSC surface area.

2016 ◽  
Vol 16 (7) ◽  
pp. 4569-4577 ◽  
Author(s):  
Tobias Wegner ◽  
Michael C. Pitts ◽  
Lamont R. Poole ◽  
Ines Tritscher ◽  
Jens-Uwe Grooß ◽  
...  

Abstract. In the Arctic polar vortex of the 2009/10 winter temperatures were low enough to allow widespread formation of polar stratospheric clouds (PSCs). These clouds occurred during the initial chlorine activation phase which provided the opportunity to investigate the impact of PSCs on chlorine activation. Satellite observations of gas-phase species and PSCs are used in combination with trajectory modeling to assess this initial activation. The initial activation occurred in association with the formation of PSCs over the east coast of Greenland at the beginning of January 2010. Although this area of PSCs covered only a small portion of the vortex, it was responsible for almost the entire initial activation of chlorine vortex wide. Observations show HCl (hydrochloric acid) mixing ratios decreased rapidly in and downstream of this region. Trajectory calculations and simplified heterogeneous chemistry modeling confirmed that the initial chlorine activation continued until ClONO2 (chlorine nitrate) was completely depleted and the activated air masses were advected throughout the polar vortex. For the calculation of heterogeneous reaction rates, surface area density is estimated from backscatter observations. Modeled heterogeneous reaction rates along trajectories intersecting with the PSCs indicate that the initial phase of chlorine activation occurred in just a few hours. These calculations also indicate that chlorine activation on the binary background aerosol is significantly slower than on the PSC particles and the observed chlorine activation can only be explained by an increase in surface area density due to PSC formation. Furthermore, there is a strong correlation between the magnitude of the observed HCl depletion and PSC surface area density.


2003 ◽  
Vol 3 (3) ◽  
pp. 839-849 ◽  
Author(s):  
P. Konopka ◽  
J.-U. Grooß ◽  
S. Bausch ◽  
R. Müller ◽  
D. S. McKenna ◽  
...  

Abstract. High-resolution simulations of the chemical composition of the Arctic stratosphere during late spring 1997 and 2000 were performed with the Chemical Lagrangian Model of the Stratosphere (CLaMS). The simulations were performed for the entire northern hemisphere on two isentropic levels 450 K (~18 km) and 585 K (~24 km). The spatial distribution and the lifetime of the vortex remnants formed after the vortex breakup in May 1997 display different behavior above and below 20 km. Above 20 km, vortex remnants propagate southward (up to 40°N) and are "frozen in'' in the summer circulation without significant mixing. Below 20 km the southward propagation of the remnants is bounded by the subtropical jet. Their lifetime is shorter by a factor of 2 than that above 20 km, owing to significant stirring below this altitude. The behavior of vortex remnants formed in March 2000 is similar but, due to an earlier vortex breakup, dominated during the first 6 weeks after the vortex breakup by westerly winds, even above 20 km. Vortex remnants formed in May 1997 are characterized by large mixing ratios of HCl indicating negligible, halogen-induced ozone loss. In contrast, mid-latitude ozone loss in late boreal spring 2000 is dominated, until mid-April, by halogen-induced ozone destruction within the vortex remnants, and subsequent transport of the ozone-depleted polar air masses (dilution) into the mid-latitudes. By varying the intensity of mixing in CLaMS, the impact of mixing on the formation of ClONO2 and ozone depletion is investigated. We find that the photochemical decomposition of HNO3 and not mixing with NOx-rich mid-latitude air is the main source of NOx within the vortex remnants in March and April 2000. Ozone depletion in the remnants is driven by ClOx photolytically formed from ClONO2. At the end of May 1997, the halogen-induced ozone deficit at 450 K poleward of 30°N amounts to ~12% with ~10% in the polar vortex and ~2% in well-isolated vortex remnants after the vortex breakup.


2013 ◽  
Vol 13 (9) ◽  
pp. 24171-24222 ◽  
Author(s):  
L. Cao ◽  
H. Sihler ◽  
U. Platt ◽  
E. Gutheil

Abstract. In recent years, the role of halogen species (e.g. Br, Cl) in the troposphere of polar regions is investigated after the discovery of their importance for boundary layer ozone destruction in the polar spring. Halogen species take part in an auto-catalytic chemical cycle including key self reactions. In this study, several chemical reaction schemes are investigated, and the importance of specific reactions and their rate constants is identified by a sensitivity analysis. A category of heterogeneous reactions related to HOBr activate halogen ions from sea salt aerosols, fresh sea ice or snow pack, driving the "bromine explosion". In the Arctic, a small amount of NOx may exist, which comes from nitrate contained in the snow, and this NOx may have a strong impact on ozone depletion. The heterogeneous reaction rates are parameterized by considering the aerodynamic resistance, a reactive surface ratio, β, i.e. ratio of reactive surface area to total ground surface area, and the boundary layer height, Lmix. It is found that for β = 1, the ozone depletion process starts after five days and lasts for 40 h for Lmix = 200 m. Ozone depletion duration becomes independent of the height of the boundary layer for about β≥20, and it approaches a value of two days for β=100. The role of nitrogen and chlorine containing species on the ozone depletion rate is studied. The calculation of the time integrated bromine and chlorine atom concentrations suggests a value in the order of 103 for the [Br] / [Cl] ratio, which reveals that atomic chlorine radicals have minor direct influence on the ozone depletion. The NOx concentrations are influenced by different chemical cycles over different time periods. During ozone depletion, the reaction cycle involving the BrONO2 hydrolysis is dominant. A critical value of 0.002 of the uptake coefficient of the BrONO2 hydrolysis reaction at the aerosol and saline surfaces is identified, beyond which the existence of NOx species accelerate the ozone depletion event – for lower values, deceleration occurs.


2018 ◽  
Vol 18 (5) ◽  
pp. 3147-3171 ◽  
Author(s):  
Scarlet Stadtler ◽  
David Simpson ◽  
Sabine Schröder ◽  
Domenico Taraborrelli ◽  
Andreas Bott ◽  
...  

Abstract. The impact of six heterogeneous gas–aerosol uptake reactions on tropospheric ozone and nitrogen species was studied using two chemical transport models, the Meteorological Synthesizing Centre-West of the European Monitoring and Evaluation Programme (EMEP MSC-W) and the European Centre Hamburg general circulation model combined with versions of the Hamburg Aerosol Model and Model for Ozone and Related chemical Tracers (ECHAM-HAMMOZ). Species undergoing heterogeneous reactions in both models include N2O5, NO3, NO2, O3, HNO3, and HO2. Since heterogeneous reactions take place at the aerosol surface area, the modelled surface area density (Sa) of both models was compared to a satellite product retrieving the surface area. This comparison shows a good agreement in global pattern and especially the capability of both models to capture the extreme aerosol loadings in east Asia. The impact of the heterogeneous reactions was evaluated by the simulation of a reference run containing all heterogeneous reactions and several sensitivity runs. One reaction was turned off in each sensitivity run to compare it with the reference run. The analysis of the sensitivity runs confirms that the globally most important heterogeneous reaction is the one of N2O5. Nevertheless, NO2, HNO3, and HO2 heterogeneous reactions gain relevance particularly in east Asia due to the presence of high NOx concentrations and high Sa in the same region. The heterogeneous reaction of O3 itself on dust is of minor relevance compared to the other heterogeneous reactions. The impacts of the N2O5 reactions show strong seasonal variations, with the biggest impacts on O3 in springtime when photochemical reactions are active and N2O5 levels still high. Evaluation of the models with northern hemispheric ozone surface observations yields a better agreement of the models with observations in terms of concentration levels, variability, and temporal correlations at most sites when the heterogeneous reactions are incorporated. Our results are loosely consistent with results from earlier studies, although the magnitude of changes induced by N2O5 reaction is at the low end of estimates, which seems to fit a trend, whereby the more recent the study the lower the impacts of these reactions.


2017 ◽  
Author(s):  
Scarlet Stadtler ◽  
David Simpson ◽  
Sabine Schröder ◽  
Domenico Taraborrelli ◽  
Andreas Bott ◽  
...  

Abstract. The impact of six heterogeneous gas-aerosol uptake reactions on tropospheric ozone and nitrogen species was studied using two chemical transport models, EMEP MSC-W and ECHAM-HAMMOZ. Species undergoing heterogeneous reactions in both models include N2O5, NO3, NO2, O3, HNO3 and HO2. Since heterogeneous reactions take place at the aerosol surface area, the modeled surface area density Sa of both models was compared to a satellite product retrieving the surface area. This comparison shows a good agreement in global pattern and especially the capability of both models to capture the extreme aerosol loadings in East Asia. The impact of the heterogeneous reactions was evaluated by the simulation of a reference run containing all heterogeneous reactions and several sensitivity runs. One reaction was turned off in each sensitivity run to compare it with the reference run. The analysis of the sensitivity runs confirms that the globally most important heterogeneous reaction is the one of N2O5. Nevertheless, NO2, HNO3 and HO2 heterogeneous reaction gain relevance particularly in East Asia due to the presence of high NOx concentrations and high Sa in the same region, although ECHAM-HAMMOZ showed much stronger responses than EMEP in this respect. The heterogeneous reaction of O3 itself on dust is of minor relevance compared to the other heterogeneous reactions. The impacts of the N2O5 reactions show strong seasonal variations, with biggest impacts on O3 in spring time when photochemical reactions are active and N2O5 levels still high. Evaluation of the models with northern hemispheric ozone surface observations yields a better agreement of the models with observations in terms of concentration levels, variability, and temporal correlations at most sites when the heterogeneous reactions are incorporated.


2019 ◽  
Vol 19 (21) ◽  
pp. 13681-13699 ◽  
Author(s):  
Marleen Braun ◽  
Jens-Uwe Grooß ◽  
Wolfgang Woiwode ◽  
Sören Johansson ◽  
Michael Höpfner ◽  
...  

Abstract. The Arctic winter 2015–2016 was characterized by exceptionally low stratospheric temperatures, favouring the formation of polar stratospheric clouds (PSCs) from mid-December until the end of February down to low stratospheric altitudes. Observations by GLORIA (Gimballed Limb Observer for Radiance Imaging of the Atmosphere) on HALO (High Altitude and LOng range research aircraft) during the PGS (POLSTRACC–GW-LCYCLE II–SALSA) campaign from December 2015 to March 2016 allow the investigation of the influence of denitrification on the lowermost stratosphere (LMS) with a high spatial resolution. Two-dimensional vertical cross sections of nitric acid (HNO3) along the flight track and tracer–tracer correlations derived from the GLORIA observations document detailed pictures of wide-spread nitrification of the Arctic LMS during the course of an entire winter. GLORIA observations show large-scale structures and local fine structures with enhanced absolute HNO3 volume mixing ratios reaching up to 11 ppbv at altitudes of 13 km in January and nitrified filaments persisting until the middle of March. Narrow coherent structures tilted with altitude of enhanced HNO3, observed in mid-January, are interpreted as regions recently nitrified by sublimating HNO3-containing particles. Overall, extensive nitrification of the LMS between 5.0 and 7.0 ppbv at potential temperature levels between 350 and 380 K is estimated. The GLORIA observations are compared with CLaMS (Chemical Lagrangian Model of the Stratosphere) simulations. The fundamental structures observed by GLORIA are well reproduced, but differences in the fine structures are diagnosed. Further, CLaMS predominantly underestimates the spatial extent of HNO3 maxima derived from the GLORIA observations as well as the overall nitrification of the LMS. Sensitivity simulations with CLaMS including (i) enhanced sedimentation rates in case of ice supersaturation (to resemble ice nucleation on nitric acid trihydrate (NAT)), (ii) a global temperature offset, (iii) modified growth rates (to resemble aspherical particles with larger surfaces) and (iv) temperature fluctuations (to resemble the impact of small-scale mountain waves) slightly improved the agreement with the GLORIA observations of individual flights. However, no parameter could be isolated which resulted in a general improvement for all flights. Still, the sensitivity simulations suggest that details of particle microphysics play a significant role for simulated LMS nitrification in January, while air subsidence, transport and mixing become increasingly important for the simulated HNO3 distributions towards the end of the winter.


2019 ◽  
Vol 19 (15) ◽  
pp. 10303-10317 ◽  
Author(s):  
Yuke Wang ◽  
Valerii Shulga ◽  
Gennadi Milinevsky ◽  
Aleksey Patoka ◽  
Oleksandr Evtushevsky ◽  
...  

Abstract. The impact of a major sudden stratospheric warming (SSW) in the Arctic in February 2018 on the midlatitude mesosphere is investigated by performing the microwave radiometer measurements of carbon monoxide (CO) and zonal wind above Kharkiv, Ukraine (50.0∘ N, 36.3∘ E). The mesospheric peculiarities of this SSW event were observed using a recently designed and installed microwave radiometer in eastern Europe for the first time. Data from the ERA-Interim and MERRA-2 reanalyses, as well as the Aura microwave limb sounder measurements, are also used. Microwave observations of the daily CO profiles in January–March 2018 allowed for the retrieval of mesospheric zonal wind at 70–85 km (below the winter mesopause) over the Kharkiv site. Reversal of the mesospheric westerly from about 10 m s−1 to an easterly wind of about −10 m s−1 around 10 February was observed. The local microwave observations at our Northern Hemisphere (NH) midlatitude site combined with reanalysis data show wide-ranging daily variability in CO, zonal wind, and temperature in the mesosphere and stratosphere during the SSW of 2018. The observed local CO variability can be explained mainly by horizontal air mass redistribution due to planetary wave activity. Replacement of the CO-rich polar vortex air by CO-poor air of the surrounding area led to a significant mesospheric CO decrease over the station during the SSW and fragmentation of the vortex over the station at the SSW start caused enhanced stratospheric CO at about 30 km. The results of microwave measurements of CO and zonal wind in the midlatitude mesosphere at 70–85 km altitudes, which still are not adequately covered by ground-based observations, are useful for improving our understanding of the SSW impacts in this region.


2018 ◽  
Author(s):  
Laura Thölix ◽  
Alexey Karpechko ◽  
Leif Backman ◽  
Rigel Kivi

Abstract. Stratospheric water vapor plays a key role in radiative and chemical processes, it e.g. influences the chemical ozone loss via controlling the polar stratospheric cloud formation in the polar stratosphere. The amount of water entering the stratosphere through the tropical tropopause differs substantially between chemistry-climate models. This is because the present-day models have difficulties in capturing the whole complexity of processes that control the water transport across the tropopause. As a result there are large differences in the stratospheric water vapour between the models. In this study we investigate the sensitivity of simulated Arctic ozone loss to the amount of water, which enters the stratosphere through the tropical tropopause. We used a chemical transport model, FinROSE-CTM, forced by ERA-Interim meteorology. The water vapour concentration in the tropical tropopause was varied between 0.5 and 1.6 times the concentration in ERA-Interim, which is similar to the range seen in chemistry climate models. The water vapour changes in the tropical tropopause led to about 1.5 and 2 ppm more water vapour in the Arctic polar vortex compared to the ERA-Interim, respectively. We found that the impact of water vapour changes on ozone loss in the Arctic polar vortex depend on the meteorological conditions. Polar stratospheric clouds form in the cold conditions within the Arctic vortex, and chlorine activation on their surface lead to ozone loss. If the cold conditions persist long enough (e.g. in 2010/11), the chlorine activation is nearly complete. In this case addition of water vapour to the stratosphere increased the formation of ICE clouds, but did not increase the chlorine activation and ozone destruction significantly. In the warm winter 2012/13 the impact of water vapour concentration on ozone loss was small, because the ozone loss was mainly NOx induced. In intermediately cold conditions, e.g. 2013/14, the effect of added water vapour was more prominent than in the other studied winters. The results show that the simulated water vapour concentration in the tropical tropopause has a significant impact on the Arctic ozone loss and deserves attention in order to improve future projections of ozone layer recovery.


2019 ◽  
Author(s):  
Marleen Braun ◽  
Jens-Uwe Grooß ◽  
Wolfgang Woiwode ◽  
Sören Johansson ◽  
Michael Höpfner ◽  
...  

Abstract. The Arctic winter 2015/16 was characterized by exceptionally cold stratospheric temperatures, favouring the formation of polar stratospheric clouds (PSCs) from mid-December until the end of February down to low stratospheric altitudes. Observations by GLORIA (Gimballed Limb Observer for Radiance Imaging of the Atmosphere) on HALO (High Altitude and LOng range research aircraft) during the PGS (POLSTRACC/GW-LCYLCE II/SALSA) campaign from December 2015 to March 2016 allow an investigation of the influence of denitrification on the lowermost stratosphere (LMS) with a high spatial resolution. For the first time vertical cross-sections of nitric acid (HNO3) along the flight track and tracer-tracer correlations derived from the GLORIA observations document detailed pictures of wide-spread nitrification of the Arctic LMS during the course of an entire winter. GLORIA observations show large-scale structures and local fine structures with strongly enhanced absolute HNO3 volume mixing ratios reaching up to 11 ppbv at altitudes of 11 km in January and nitrified filaments persisting until the middle of March. Narrow streaks of enhanced HNO3, observed in mid-January, are interpreted as regions recently nitrified by sublimating HNO3-containing particles. Overall, a nitrification of the LMS between 5.0 ppbv and 7.0 ppbv at potential temperature levels between 350 and 380 K is estimated. This extent of nitrification has never been observed before in the Arctic lowermost stratosphere. The GLORIA observations are compared with CLaMS (Chemical Lagrangian Model of the Stratosphere) simulations. The fundamental structures observed by GLORIA are well reproduced, but differences in the fine structures are diagnosed. Further, CLaMS predominantly underestimates the spatial extent of maximum HNO3 mixing ratios derived from the GLORIA observations as well as the enhancement at lower altitudes. Sensitivity simulations with CLaMS including (i) enhanced sedimentation rates in case of ice supersaturation (to resemble ice nucleation on NAT), (ii) a global temperature offset, (iii) modified growth rates (to resemble aspherical particles with larger surfaces) and (iv) temperature fluctuations (to resemble the impact of small-scale mountain waves) mostly improve the agreement with the GLORIA observations. The sensitivity simulations suggest that details of particle microphysics play a significant role for simulated LMS nitrification in January, while air subsidence, transport and mixing become increasingly important towards the end of the winter.


2009 ◽  
Vol 22 (23) ◽  
pp. 6168-6180 ◽  
Author(s):  
A. G. Marshall ◽  
A. A. Scaife ◽  
S. Ineson

Abstract The impact of explosive volcanic eruptions on the atmospheric circulation at high northern latitudes is assessed in two versions of the Met Office Hadley Centre’s atmospheric climate model. The standard version of the model extends to an altitude of around 40 km, while the extended version has enhanced stratospheric resolution and reaches 85-km altitude. Seasonal hindcasts initialized on 1 December produce a strengthening of the winter polar vortex and anomalous warming over northern Europe characteristic of the positive phase of the Arctic Oscillation (AO) when forced with volcanic aerosol following the 1963 Mount Agung, 1982 El Chichón, and 1991 Mount Pinatubo eruptions, as is observed. The AO signal in the extended model is of comparable strength to that in the standard model, showing that there is little impact from both increasing the vertical resolution in the stratosphere and extending the model domain to near the mesopause. The presence of this signal in the models, however, is likely due to the persistence of the observed signal from the initial conditions, because a similar set of experiments initiated with the same conditions, but with no volcanic aerosol forcing, exhibits a similar response as the forced runs. This suggests that the model has limited fidelity in capturing the response to volcanic aerosols on its own, consistent with previous studies on the impact of volcanic forcing in long climate simulations, but does support the premise that seasonal winter forecasts are substantially improved with the inclusion of stratospheric information.


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