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 ◽  
...  

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.

2015 ◽  
Vol 15 (4) ◽  
pp. 5391-5422
Author(s):  
G. Wetzel ◽  
H. Oelhaf ◽  
M. Birk ◽  
A. de Lange ◽  
A. Engel ◽  
...  

Abstract. The Arctic winter 2010/11 was characterized by a persisting vortex with extremely cold 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. MIPAS (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 is 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 in the stratosphere has been derived by combining MIPAS-B and TELIS simultaneously observed molecules. A total chlorine amount of 3.41 ± 0.30 ppbv is inferred from the measurements. This value is in line with previously carried out stratospheric observations confirming the slightly decreasing chlorine trend 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 observation taking into account the fact that some chlorine source gases and very short lived species are not included in the model.


2017 ◽  
Author(s):  
Gerald Wetzel ◽  
Hermann Oelhaf ◽  
Michael Höpfner ◽  
Felix Friedl-Vallon ◽  
Andreas Ebersoldt ◽  
...  

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.


2017 ◽  
Vol 17 (23) ◽  
pp. 14631-14643
Author(s):  
Gerald Wetzel ◽  
Hermann Oelhaf ◽  
Michael Höpfner ◽  
Felix Friedl-Vallon ◽  
Andreas Ebersoldt ◽  
...  

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.


Author(s):  
Yousuke Yamashita ◽  
Hideharu Akiyoshi ◽  
Masaaki Takahashi

Arctic ozone amount in winter to spring shows large year-to-year variation. This study investigates Arctic spring ozone in relation to the phase of quasi-biennial oscillation (QBO)/the 11-year solar cycle, using satellite observations, reanalysis data, and outputs of a chemistry climate model (CCM) during the period of 1979–2011. For this duration, we found that the composite mean of the Northern Hemisphere high-latitude total ozone in the QBO-westerly (QBO-W)/solar minimum (Smin) phase is slightly smaller than those averaged for the QBO-W/Smax and QBO-E/Smax years in March. An analysis of a passive ozone tracer in the CCM simulation indicates that this negative anomaly is primarily caused by transport. The negative anomaly is consistent with a weakening of the residual mean downward motion in the polar lower stratosphere. The contribution of chemical processes estimated using the column amount difference between ozone and the passive ozone tracer is between 10–20% of the total anomaly in March. The lower ozone levels in the Arctic spring during the QBO-W/Smin years are associated with a stronger Arctic polar vortex from late winter to early spring, which is linked to the reduced occurrence of sudden stratospheric warming in the winter during the QBO-W/Smin years.


2019 ◽  
Author(s):  
Hideaki Nakajima ◽  
Isao Murata ◽  
Yoshihiro Nagahama ◽  
Hideharu Akiyoshi ◽  
Kosuke Saeki ◽  
...  

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.


2012 ◽  
Vol 12 (14) ◽  
pp. 6581-6592 ◽  
Author(s):  
G. Wetzel ◽  
H. Oelhaf ◽  
O. Kirner ◽  
F. Friedl-Vallon ◽  
R. Ruhnke ◽  
...  

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.


2018 ◽  
Author(s):  
Farahnaz Khosrawi ◽  
Oliver Kirner ◽  
Gabriele Stiller ◽  
Michael Höpfner ◽  
Michelle L. Santee ◽  
...  

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.


Atmosphere ◽  
2021 ◽  
Vol 12 (5) ◽  
pp. 582
Author(s):  
Yousuke Yamashita ◽  
Hideharu Akiyoshi ◽  
Masaaki Takahashi

Arctic ozone amount in winter to spring shows large year-to-year variation. This study investigates Arctic spring ozone in relation to the phase of quasi-biennial oscillation (QBO)/the 11-year solar cycle, using satellite observations, reanalysis data, and outputs of a chemistry climate model (CCM) during the period of 1979–2017. For this duration, we found that the composite mean of the Northern Hemisphere high-latitude total ozone in the QBO-westerly (QBO-W)/solar minimum (Smin) phase is slightly smaller than those averaged for the QBO-W/Smax and QBO-E/Smax years in March. An analysis of a passive ozone tracer in the CCM simulation indicates that this negative anomaly is primarily caused by transport. The negative anomaly is consistent with a weakening of the residual mean downward motion in the polar lower stratosphere. The contribution of chemical processes estimated using the column amount difference between ozone and the passive ozone tracer is between 10–20% of the total anomaly in March. The lower ozone levels in the Arctic spring during the QBO-W/Smin years are associated with a stronger Arctic polar vortex from late winter to early spring, which is linked to the reduced occurrence of sudden stratospheric warming in the winter during the QBO-W/Smin years.


2018 ◽  
Vol 18 (12) ◽  
pp. 8873-8892 ◽  
Author(s):  
Farahnaz Khosrawi ◽  
Oliver Kirner ◽  
Gabriele Stiller ◽  
Michael Höpfner ◽  
Michelle L. Santee ◽  
...  

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.


2012 ◽  
Vol 12 (2) ◽  
pp. 4867-4900
Author(s):  
G. Wetzel ◽  
H. Oelhaf ◽  
F. Friedl-Vallon ◽  
O. Kirner ◽  
A. Kleinert ◽  
...  

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.


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