scholarly journals Diurnal variations of BrONO<sub>2</sub> observed by MIPAS-B at mid-latitudes and in the Arctic

2017 ◽  
Author(s):  
Gerald Wetzel ◽  
Hermann Oelhaf ◽  
Michael Höpfner ◽  
Felix Friedl-Vallon ◽  
Andreas Ebersoldt ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Climate Model ◽  
Michelson Interferometer ◽  
Diurnal Variations ◽  
The Arctic ◽  
Late Winter ◽  
Mixing Ratios ◽  
Reservoir Species ◽  
Atmospheric Sounding ◽  
Stratospheric Clouds

Abstract. The first stratospheric measurements of the diurnal variation of the inorganic bromine (Bry) reservoir species BrONO2 around sunrise and sunset are reported. Arctic flights of the balloon-borne Michelson Interferometer for Passive Atmospheric Sounding (MIPAS-B) were carried out from Kiruna (68°N, Sweden) in January 2010 and March 2011 inside the stratospheric polar vortices where diurnal variations of BrONO2 around sunrise have been observed. High nighttime BrONO2 volume mixing ratios of up to 21 parts per trillion by volume (pptv) were detected in the late winter 2011 in the absence of polar stratospheric clouds (PSCs). In contrast, the amount of measured BrONO2 was significantly lower in January 2010 due to low available NO2 amounts (for the build-up of BrONO2), heterogeneous destruction of BrONO2 on PSC particles, and the gas-phase interaction of BrO (the source to form BrONO2) with ClO. A further balloon flight took place at mid-latitudes from Timmins (49°N, Canada) in September 2014. Mean BrONO2 mixing ratios of 22 pptv were observed after sunset in the altitude region between 21 and 29 km. Measurements are compared and discussed with the results of a multi-year simulation performed with the chemistry climate model ECHAM5/MESSy Atmospheric Chemistry (EMAC). The calculated temporal variation of BrONO2 is in principal agreement with the balloon-borne observations. Using the nighttime simulated ratio between BrONO2 and Bry, the amount of Bry observed by MIPAS-B was estimated to about 21–25 pptv in the lower stratosphere.

scholarly journals Diurnal variations of BrONO<sub>2</sub> observed by MIPAS-B at midlatitudes and in the Arctic

2017 ◽  
Vol 17 (23) ◽  
pp. 14631-14643
Author(s):  
Gerald Wetzel ◽  
Hermann Oelhaf ◽  
Michael Höpfner ◽  
Felix Friedl-Vallon ◽  
Andreas Ebersoldt ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Climate Model ◽  
Michelson Interferometer ◽  
Diurnal Variations ◽  
The Arctic ◽  
Late Winter ◽  
Mixing Ratios ◽  
Reservoir Species ◽  
Atmospheric Sounding ◽  
Stratospheric Clouds

Abstract. The first stratospheric measurements of the diurnal variation in the inorganic bromine (Bry) reservoir species BrONO2 around sunrise and sunset are reported. Arctic flights of the balloon-borne Michelson Interferometer for Passive Atmospheric Sounding (MIPAS-B) were carried out from Kiruna (68° N, Sweden) in January 2010 and March 2011 inside the stratospheric polar vortices where diurnal variations of BrONO2 around sunrise have been observed. High nighttime BrONO2 volume mixing ratios of up to 21 pptv (parts per trillion by volume) were detected in late winter 2011 in the absence of polar stratospheric clouds (PSCs). In contrast, the amount of measured BrONO2 was significantly lower in January 2010 due to low available NO2 amounts (for the build-up of BrONO2), the heterogeneous destruction of BrONO2 on PSC particles, and the gas-phase interaction of BrO (the source to form BrONO2) with ClO. A further balloon flight took place at midlatitudes from Timmins (49° N, Canada) in September 2014. Mean BrONO2 mixing ratios of 22 pptv were observed after sunset in the altitude region between 21 and 29 km. Measurements are compared and discussed with the results of a multi-year simulation performed with the chemistry climate model ECHAM5/MESSy Atmospheric Chemistry (EMAC). The calculated temporal variation in BrONO2 largely reproduces the balloon-borne observations. Using the nighttime simulated ratio between BrONO2 and Bry, the amount of Bry observed by MIPAS-B was estimated to be about 21–25 pptv in the lower stratosphere.

scholarly journals Diurnal variations of reactive chlorine and nitrogen oxides observed by MIPAS-B inside the January 2010 Arctic vortex

2012 ◽  
Vol 12 (14) ◽  
pp. 6581-6592 ◽  
Author(s):  
G. Wetzel ◽  
H. Oelhaf ◽  
O. Kirner ◽  
F. Friedl-Vallon ◽  
R. Ruhnke ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Climate Model ◽  
Michelson Interferometer ◽  
Emission Spectra ◽  
The Arctic ◽  
Polar Stratospheric Clouds ◽  
Model Calculations ◽  
Mixing Ratios ◽  
Reservoir Species ◽  
Stratospheric Clouds

Abstract. The winter 2009/2010 was characterized by a strong Arctic vortex with extremely cold mid-winter temperatures in the lower stratosphere associated with an intense activation of reactive chlorine compounds (ClOx) from reservoir species. Stratospheric limb emission spectra were recorded during a flight of the balloon version of the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS-B) from Kiruna (Sweden) on 24 January 2010 inside the Arctic vortex. Several fast limb sequences of spectra (in time steps of about 10 min) were measured from nighttime photochemical equilibrium to local noon allowing the retrieval of chlorine- and nitrogen-containing species which change rapidly their concentration around the terminator between night and day. Mixing ratios of species like ClO, NO2, and N2O5 show significant changes around sunrise, which are temporally delayed due to polar stratospheric clouds reducing the direct radiative flux from the sun. ClO variations were derived for the first time from MIPAS-B spectra. Daytime ClO values of up to 1.6 ppbv are visible in a broad chlorine activated layer below 26 km correlated with low values (below 0.1 ppbv) of the chlorine reservoir species ClONO2. Observations are compared and discussed with calculations performed with the 3-dimensional Chemistry Climate Model EMAC (ECHAM5/MESSy Atmospheric Chemistry). Mixing ratios of the species ClO, NO2, and N2O5 are well reproduced by the model during night and noon. However, the onset of ClO production and NO2 loss around the terminator in the model is not consistent with the measurements. The MIPAS-B observations along with Tropospheric Ultraviolet-Visible (TUV) radiation model calculations suggest that polar stratospheric clouds lead to a delayed start followed by a faster increase of the photodissoziation of ClOOCl and NO2 near the morning terminator since stratospheric clouds alter the direct and the diffuse flux of solar radiation. These effects are not considered in the EMAC model simulations which assume a cloudless atmosphere.

scholarly journals Total depletion of ozone reached in the 2010–2011 Arctic winter as observed by MIPAS/ENVISAT using a 2-D tomographic approach

2011 ◽  
Vol 11 (12) ◽  
pp. 33191-33227
Author(s):  
E. Arnone ◽  
E. Castelli ◽  
E. Papandrea ◽  
M. Carlotti ◽  
B. M. Dinelli
Keyword(s):  
Potential Temperature ◽  
Michelson Interferometer ◽  
The Arctic ◽  
Late Winter ◽  
Infrared Measurements ◽  
Atmospheric Sounding ◽  
Depletion Rate ◽  
Horizontal Inhomogeneity ◽  
Stratospheric Clouds ◽  
The Antarctic

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. Through inspection of MIPAS spectra, 84% of PSCs were identified as supercooled ternary solution (STS) or STS mixed with nitric acid trihydrate (NAT), 16% formed mostly by NAT particles, and only a few 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. Sporadic increases of NO2 associated with evaporation of sedimenting PSCs were also observed. Once the PSC season halted, ClO was reconverted 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.

scholarly journals Comparison of ECHAM5/MESSy Atmospheric Chemistry (EMAC) simulations of the Arctic winter 2009/2010 and 2010/2011 with Envisat/MIPAS and Aura/MLS observations

2018 ◽  
Vol 18 (12) ◽  
pp. 8873-8892 ◽  
Author(s):  
Farahnaz Khosrawi ◽  
Oliver Kirner ◽  
Gabriele Stiller ◽  
Michael Höpfner ◽  
Michelle L. Santee ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Climate Model ◽  
Michelson Interferometer ◽  
Volume Density ◽  
The Arctic ◽  
Model Simulations ◽  
Vertical Extension ◽  
Realistic Representation ◽  
Set Up ◽  
Stratospheric Clouds

Abstract. We present model simulations with the atmospheric chemistry–climate model ECHAM5/MESSy Atmospheric Chemistry (EMAC) nudged toward European Centre for Medium-Range Weather Forecasts (ECMWF) ERA-Interim reanalyses for the Arctic winters 2009/2010 and 2010/2011. This study is the first to perform an extensive assessment of the performance of the EMAC model for Arctic winters as previous studies have only made limited evaluations of EMAC simulations which also were mainly focused on the Antarctic winter stratosphere. We have chosen the two extreme Arctic winters 2009/2010 and 2010/2011 to evaluate the formation of polar stratospheric clouds (PSCs) and the representation of the chemistry and dynamics of the polar winter stratosphere in EMAC. The EMAC simulations are compared to observations by the Michelson Interferometer for Passive Atmospheric Soundings (Envisat/MIPAS) and the observations from the Aura Microwave Limb Sounder (Aura/MLS). The Arctic winter 2010/2011 was one of the coldest stratospheric winters on record, leading to the strongest depletion of ozone measured in the Arctic. The Arctic winter 2009/2010 was, from the climatological perspective, one of the warmest stratospheric winters on record. However, it was distinguished by an exceptionally cold stratosphere (colder than the climatological mean) from mid-December 2009 to mid-January 2010, leading to prolonged PSC formation and existence. Significant denitrification, the removal of HNO3 from the stratosphere by sedimentation of HNO3-containing polar stratospheric cloud particles, occurred in that winter. In our comparison, we focus on PSC formation and denitrification. The comparisons between EMAC simulations and satellite observations show that model and measurements compare well for these two Arctic winters (differences for HNO3 generally within ±20 %) and thus that EMAC nudged toward ECMWF ERA-Interim reanalyses is capable of giving a realistic representation of the evolution of PSCs and associated sequestration of gas-phase HNO3 in the polar winter stratosphere. However, simulated PSC volume densities are smaller than the ones derived from Envisat/MIPAS observations by a factor of 3–7. Further, PSCs in EMAC are not simulated as high up (in altitude) as they are observed. This underestimation of PSC volume density and vertical extension of the PSCs results in an underestimation of the vertical redistribution of HNO3 due to denitrification/re-nitrification. The differences found here between model simulations and observations stipulate further improvements in the EMAC set-up for simulating PSCs.

scholarly journals Diurnal variations of reactive chlorine and nitrogen oxides observed by MIPAS-B inside the January 2010 Arctic vortex

2012 ◽  
Vol 12 (2) ◽  
pp. 4867-4900
Author(s):  
G. Wetzel ◽  
H. Oelhaf ◽  
F. Friedl-Vallon ◽  
O. Kirner ◽  
A. Kleinert ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Lower Stratosphere ◽  
Climate Model ◽  
Michelson Interferometer ◽  
Emission Spectra ◽  
The Arctic ◽  
Mixing Ratios ◽  
Simulated Concentration ◽  
Concentration Changes ◽  
Night And Day

Abstract. The winter 2009/2010 was characterized by a strong Arctic vortex with extremely cold mid-winter temperatures in the lower stratosphere associated with an intense activation of reactive chlorine compounds (ClOx). In order to assess the capacities of state-of-the-art chemistry models to predict polar stratospheric chemistry, stratospheric limb emission spectra were recorded during a flight of the balloon version of the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS-B) from Kiruna (Sweden) on 24 January 2010 inside the Arctic vortex. Several fast limb sequences of spectra (in time steps of about 10 min) were measured from nighttime photochemical equilibrium to local noon allowing the retrieval of chlorine- and nitrogen-containing species which change quickly their concentration around the terminator between night and day. Mixing ratios of species like ClO, NO2, and N2O5 show significant changes around sunrise, which are temporally delayed due to shadowing of the lower stratosphere by upper tropospheric and polar stratospheric clouds. ClO variations were derived for the first time from MIPAS-B spectra. Daytime ClO values of up to 1.6 ppbv are visible in a broad chlorine activated layer below 26 km correlated with low values (close to zero) of its reservoir species ClONO2. Observations are compared and discussed with calculations performed with the 3-dimensional Chemistry Climate Model EMAC (ECHAM5/MESSy Atmospheric Chemistry). Mixing ratios of the species ClO, NO2, and N2O5 are fairly well reproduced by the model during photochemical equilibrium. However, since the model assumes cloudless illumination, simulated concentration changes around sunrise start earlier but less quickly compared to the observed variation of the species concentration.

scholarly journals Partitioning and budget of inorganic and organic chlorine species observed by MIPAS-B and TELIS in the Arctic in March 2011

2015 ◽  
Vol 15 (14) ◽  
pp. 8065-8076 ◽  
Author(s):  
G. Wetzel ◽  
H. Oelhaf ◽  
M. Birk ◽  
A. de Lange ◽  
A. Engel ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Climate Model ◽  
Michelson Interferometer ◽  
Polar Vortex ◽  
The Arctic ◽  
Late Winter ◽  
Winter Solstice ◽  
Organic Chlorine ◽  
The Tropics ◽  
Inorganic And Organic

Abstract. The Arctic winter 2010/2011 was characterized by a persistent vortex with extremely low temperatures in the lower stratosphere above northern Scandinavia leading to a strong activation of chlorine compounds (ClOx) like Cl, Cl2, ClO, ClOOCl, OClO, and HOCl, which rapidly destroyed ozone when sunlight returned after winter solstice. The MIPAS-B (Michelson Interferometer for Passive Atmospheric Sounding) and TELIS (TErahertz and submillimeter LImb Sounder) balloon measurements obtained in northern Sweden on 31 March 2011 inside the polar vortex have provided vertical profiles of inorganic and organic chlorine species as well as diurnal variations of ClO around sunrise over the whole altitude range in which chlorine has been undergoing activation and deactivation. This flight was performed at the end of the winter during the last phase of ClOx deactivation. The complete inorganic and organic chlorine partitioning and budget for 31 March 2011, assumed to be representative for the late-winter Arctic stratosphere, has been derived by combining MIPAS-B and TELIS simultaneously observed molecules. A total chlorine amount of 3.41 ± 0.30 parts per billion by volume is inferred from the measurements (above 24 km). This value is in line with previous stratospheric observations carried out outside the tropics confirming the slightly decreasing chlorine amount in the stratosphere. Observations are compared and discussed with the output of a multi-year simulation performed with the chemistry climate model EMAC (ECHAM5/MESSy Atmospheric Chemistry). The simulated stratospheric total chlorine amount is in accordance with the MIPAS-B/TELIS observations, taking into account the fact that some chlorine source gases and very short-lived species are not included in the model.

scholarly journals Chlorine partitioning near the polar vortex boundary observed with ground-based FTIR and satellites at Syowa Station, Antarctica in 2007 and 2011

2019 ◽  
Author(s):  
Hideaki Nakajima ◽  
Isao Murata ◽  
Yoshihiro Nagahama ◽  
Hideharu Akiyoshi ◽  
Kosuke Saeki ◽  
...  
Keyword(s):  
Temporal Variation ◽  
Negative Correlation ◽  
Climate Model ◽  
Michelson Interferometer ◽  
Polar Vortex ◽  
The Arctic ◽  
Additional Increase ◽  
Syowa Station ◽  
Reservoir Species ◽  
Satellite Sensor

Abstract. We retrieved lower stratospheric vertical profiles of O3, HNO3, and HCl from solar spectra taken with a ground-based Fourier-Transform infrared spectrometer (FTIR) installed at Syowa Station, Antarctica (69.0° S, 39.6° E) from March to December 2007 and September to November 2011. This was the first continuous measurements of chlorine species throughout the ozone hole period from the ground in Antarctica. We analyzed temporal variation of these species combined with ClO, HCl, and HNO3 data taken with the Aura/MLS (Microwave Limb Sounder) satellite sensor, and ClONO2 data taken with the Envisat/MIPAS (The Michelson Interferometer for Passive Atmospheric Sounding) satellite sensor at 18 and 22 km over Syowa Station. HCl and ClONO2 decrease occurred at both 18 and 22 km, and soon ClONO2 was almost depleted in early winter. When the sun returned to Antarctica in spring, enhancement of ClO and gradual O3 destruction were observed. During the ClO enhanced period, negative correlation between ClO and ClONO2 was observed in the time-series of the data at Syowa Station. This negative correlation was associated with the distance between Syowa Station and the inner edge of the polar vortex. We used MIROC3.2 Chemistry-Climate Model (CCM) results to see the comprehensive behavior of chlorine and related species inside the polar vortex and the edge region in more detail. From CCM model results, rapid conversion of chlorine reservoir species (HCl and ClONO2) into Cl2, gradual conversion of Cl2 into Cl2O2, increase of ClO when sunlight became available, and conversion of ClO into HCl, was successfully reproduced. HCl decrease in the winter polar vortex core continued to occur due to the transport of ClONO2 from the subpolar region to higher latitudes, providing a flux of ClONO2 from more sunlit latitudes into the polar vortex. Temporal variation of chlorine species over Syowa Station was affected by both heterogeneous chemistry related to Polar Stratospheric Cloud (PSC) occurrence deep inside the polar vortex, and transport of an NOx-rich airmass from lower latitudinal polar vortex boundary region which can produce additional ClONO2 by reaction of ClO with NO2. The deactivation pathways from active chlorine into reservoir species (HCl and/or ClONO2) were found to be highly dependent on the availability of ambient O3. At an altitude where most ozone was depleted in Antarctica (18 km), most ClO was converted to HCl. However, at an altitude where there were some O3 available (22 km), additional increase of ClONO2 from initial value can occur, similar to the case in the Arctic.

scholarly journals Extreme ozone depletion in the 2010–2011 Arctic winter stratosphere as observed by MIPAS/ENVISAT using a 2-D tomographic approach

2012 ◽  
Vol 12 (19) ◽  
pp. 9149-9165 ◽  
Author(s):  
E. Arnone ◽  
E. Castelli ◽  
E. Papandrea ◽  
M. Carlotti ◽  
B. M. Dinelli
Keyword(s):  
Ozone Depletion ◽  
Potential Temperature ◽  
Michelson Interferometer ◽  
The Arctic ◽  
Late Winter ◽  
Infrared Measurements ◽  
Depletion Rate ◽  
Horizontal Inhomogeneity ◽  
Stratospheric Clouds ◽  
The Antarctic

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.

scholarly journals HOCl chemistry in the Antarctic stratospheric vortex 2002, as observed with the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS)

2008 ◽  
Vol 8 (6) ◽  
pp. 18967-18992
Author(s):  
T. von Clarmann ◽  
N. Glatthor ◽  
R. Ruhnke ◽  
G. P. Stiller ◽  
O. Kirner ◽  
...  
Keyword(s):  
Heterogeneous Reaction ◽  
Michelson Interferometer ◽  
Polar Vortex ◽  
Heterogeneous Chemistry ◽  
Polar Stratospheric Clouds ◽  
Mean Values ◽  
Mixing Ratios ◽  
Atmospheric Sounding ◽  
Antarctic Polar Vortex ◽  
Stratospheric Clouds

Abstract. In the 2002 Antarctic polar vortex enhanced HOCl mixing ratios were detected by the Michelson Interferometer for Passive Atmospheric Sounding both at altitudes of around 35 km, where HOCl abundances are ruled by gas phase chemistry and at around 24 km, which belongs to the altitude domain where heterogeneous chlorine chemistry is relevant. At altitudes of 33 to 40 km, where in midlatitudinal and tropical atmospheres peak HOCl mixing ratios significantly above 0.2 ppbv (in terms of daily mean values) are observed, polar vortex HOCl mixing ratios were found to be around 0.14 ppbv as long as the polar vortex was intact, centered at the pole, and thus received relatively little sunlight. After deformation and displacement of the polar vortex in the course of a major warming, ClO rich vortex air was more exposed to sunlight, where enhanced HOx abundances led to largely increased HOCl mixing ratios (up to 0.3 ppbv), exceeding typical midlatitudinal and tropical amounts significantly. The HOCl increase was preceded by an increase of ClO. Model runs could reproduce these measurements only when the Stimpfle et al. (1979) rate constant for the reaction ClO+HO2→HOCl+O2 was used but not with the current JPL recommendation. At an altitude of 24 km, HOCl mixing ratios of up to 0.15 ppbv were detected. This HOCl enhancement, which is already visible in 18 September data, is attributed to heterogeneous chemistry, which is in agreement with observations of polar stratospheric clouds. Comparison with a model run where no polar stratospheric clouds appeared during the observation period suggests that a significant part of HOCl was generated from ClO rather than directly via heterogeneous reaction. Excess ClO and HOCl in the measurements is attributed to ongoing heterogeneous chemistry which is not reproduced by the model. In the following days, a decay of HOCl abundances was observed and on 11 October, polar vortex mean daytime mixing ratios were only 0.03 ppbv.

scholarly journals Comparison of ECHAM5/MESSy Atmospheric Chemistry (EMAC) Simulations of the Arctic winter 2009/2010 and 2010/2011 with Envisat/MIPAS and Aura/MLS Observations

2018 ◽  
Author(s):  
Farahnaz Khosrawi ◽  
Oliver Kirner ◽  
Gabriele Stiller ◽  
Michael Höpfner ◽  
Michelle L. Santee ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Climate Model ◽  
Michelson Interferometer ◽  
Volume Density ◽  
Cloud Formation ◽  
The Arctic ◽  
Cold Temperatures ◽  
Vertical Extension ◽  
Polar Stratospheric Cloud ◽  
Realistic Representation

Abstract. We present model simulations with the atmospheric chemistry-climate model ECHAM5/MESSy Atmospheric Chemistry (EMAC) nudged toward European Center for Medium-Range Weather Forecasts (ECMWF) reanalyses for the Arctic winter 2009/2010 and 2010/2011. This study is the first to perform an extensive assessment of the performance of the EMAC model for Arctic winters; previous studies have only made limited evaluations of EMAC simulations for the Arctic. We have chosen the two extreme Arctic winters 2009/2010 and 2010/2011 to evaluate the formation of polar stratospheric clouds (PSCs) and the representation of the chemistry and dynamics of the polar winter stratosphere in EMAC. The EMAC simulations are compared to observations by the Michelson Interferometer for Passive Atmospheric Soundings (Envisat/MIPAS) and the observations from the Aura Microwave Limb Sounder (Aura/MLS). The Arctic winter 2010/2011 was one of the coldest winters on record, leading to the strongest depletion of ozone measured in the Arctic. The Arctic winter 2009/2010 was, from the climatological perspective, one of the warmest winters on record. However, it was distinguished by an exceptionally cold stratosphere (colder than the climatological mean). Cold temperatures prevailed from mid December 2009 to mid January 2010, leading to prolonged PSC formation and existence. Significant denitrification, the removal of HNO3 from the stratosphere by sedimentation of HNO3 containing polar stratospheric cloud particles, occurred. In our comparison, we focus on polar stratospheric cloud formation and denitrification. The comparisons between EMAC simulations and satellite observations show that model and measurements compare well for these two Arctic winters (differences for HNO3 generally within ±20 %) and thus that EMAC nudged toward ECMWF reanalyses is capable of giving a realistic representation of the evolution of PSCs and the associated sequestration of gas-phase HNO3 in the polar winter stratosphere. However, simulated PSC volume densities are several orders of magnitude smaller than the ones derived from Envisat/MIPAS observations. Further, PSCs in EMAC are not simulated as high up as they are observed. This underestimation of PSC volume density and vertical extension of the PSCs results in an underestimation of the vertical redistribution of HNO3 due to denitrification/re-nitrification.

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