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 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 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 MIPAS detects Antarctic stratospheric belt of NAT PSCs caused by mountain waves

2005 ◽  
Vol 5 (5) ◽  
pp. 10723-10745 ◽  
Author(s):  
M. Höpfner ◽  
N. Larsen ◽  
R. Spang ◽  
B. P. Luo ◽  
J. Ma ◽  
...  
Keyword(s):  
Nitric Acid ◽  
Michelson Interferometer ◽  
Sudden Onset ◽  
Abstract Space ◽  
Mountain Waves ◽  
Homogeneous Surface ◽  
Surface Nucleation ◽  
Atmospheric Sounding ◽  
Stratospheric Clouds ◽  
The Antarctic

Abstract. Space borne infrared limb emission measurements by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) reveal the formation of a belt of polar stratospheric clouds (PSCs) of nitric acid trihydrate (NAT) particles over Antarctica in mid-June 2003. By mesoscale microphysical simulations we show that this sudden onset of NAT PSCs was caused by heterogeneous nucleation on ice in the cooling phases of large-amplitude stratospheric mountain waves over the Antarctic Peninsula and the Ellsworth Mountains. MIPAS observations of PSCs before this event show no indication for the presence of NAT clouds with volume densities larger than about 0.3 μm3/cm3 and radii smaller than 3 μm, but are consistent with supercooled droplets of ternary H2SO4/HNO3/H2O solution (STS). Simulations indicate that homogeneous surface nucleation rates have to be reduced by three orders of magnitude to comply with the observations.

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

2009 ◽  
Vol 9 (5) ◽  
pp. 1817-1829 ◽  
Author(s):  
T. von Clarmann ◽  
N. Glatthor ◽  
R. Ruhnke ◽  
G. P. Stiller ◽  
O. Kirner ◽  
...  
Keyword(s):  
Heterogeneous Reaction ◽  
Potential Temperature ◽  
Michelson Interferometer ◽  
Polar Vortex ◽  
Heterogeneous Chemistry ◽  
Polar Stratospheric Clouds ◽  
Mean Values ◽  
Mixing Ratios ◽  
Atmospheric Sounding ◽  
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 (1000 K potential temperature), where HOCl abundances are ruled by gas phase chemistry and at around 18–24 km (475–625 K), which belongs to the altitude domain where heterogeneous chlorine chemistry is relevant. At altitudes of 33 to 40 km 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. This is the altitude region where in midlatitudinal and tropic atmospheres peak HOCl mixing ratios significantly above 0.2 ppbv (in terms of daily mean values) are observed. 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. The measurements were compared to a model run where no polar stratospheric clouds appeared during the observation period. The fact that HOCl still was produced in the model run suggests that a significant part of HOCl was generated from ClO rather than directly via heterogeneous reaction. Excess ClO, lower ClONO2 and earlier loss of HOCl in the measurements are attributed to ongoing heterogeneous chemistry which is not reproduced by the model. On 11 October, polar vortex mean daytime mixing ratios were only 0.03 ppbv.

scholarly journals MIPAS detects Antarctic stratospheric belt of NAT PSCs caused by mountain waves

2006 ◽  
Vol 6 (5) ◽  
pp. 1221-1230 ◽  
Author(s):  
M. Höpfner ◽  
N. Larsen ◽  
R. Spang ◽  
B. P. Luo ◽  
J. Ma ◽  
...  
Keyword(s):  
Nitric Acid ◽  
Michelson Interferometer ◽  
Sudden Onset ◽  
Abstract Space ◽  
Mountain Waves ◽  
Homogeneous Surface ◽  
Surface Nucleation ◽  
Atmospheric Sounding ◽  
Stratospheric Clouds ◽  
The Antarctic

Abstract. Space borne infrared limb emission measurements by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) reveal the formation of a belt of polar stratospheric clouds (PSCs) of nitric acid trihydrate (NAT) particles over Antarctica in mid-June 2003. By mesoscale microphysical simulations we show that this sudden onset of NAT PSCs was caused by heterogeneous nucleation on ice in the cooling phases of large-amplitude stratospheric mountain waves over the Antarctic Peninsula and the Ellsworth Mountains. MIPAS observations of PSCs before this event show no indication for the presence of NAT clouds with volume densities larger than about 0.3 µm3/cm3 and radii smaller than 3 µm, but are consistent with supercooled droplets of ternary H2SO4/HNO3/H2O solution (STS). Simulations indicate that homogeneous surface nucleation rates have to be reduced by three orders of magnitude to comply with the observations.

scholarly journals Chemical analysis of refractory stratospheric aerosol particles collected within the arctic vortex and inside polar stratospheric clouds

2016 ◽  
Author(s):  
Martin Ebert ◽  
Ralf Weigel ◽  
Konrad Kandler ◽  
Gebhard Günther ◽  
Sergej Molleker ◽  
...  
Keyword(s):  
Aerosol Particles ◽  
Stratospheric Aerosol ◽  
The Arctic ◽  
Late Winter ◽  
General Tendency ◽  
Polar Stratospheric Clouds ◽  
Metal Mixtures ◽  
Air Masses ◽  
Size And Morphology ◽  
Stratospheric Clouds

Abstract. Stratospheric aerosol particles with diameters larger than about 10 nm were collected within the arctic vortex during two polar flight campaigns: RECONCILE in winter 2010 and ESSenCe in winter 2011. Impactors were installed on board of the aircraft M-55 Geophysica, which was operated from Kiruna, Sweden. Flights were performed in a height of up to 21 km and some of the particle samples were taken within distinct polar stratospheric clouds (PSC). The chemical composition, size and morphology of refractory particles were analyzed by scanning electron microscopy and energy-dispersive X-ray microanalysis. During ESSenCe no refractory particles with diameters above 500 nm were sampled. In total 116 small silicate-, Fe-rich-, Pb-rich and aluminum oxide spheres were found. In contrast to ESSenCe early winter, during the late winter RECONCILE mission the air masses were subsiding inside the Arctic winter vortex from upper stratosphere and mesosphere, thus initializing a transport of refractory aerosol particles into the lower stratosphere. During RECONCILE 759 refractory particles with diameters above 500 nm were found consisting of silicates, silicate/carbon mixtures, Fe-rich particles, Ca-rich particles and complex metal mixtures. In the size range below 500 nm additionally the presence of soot was proven. While the data base is still sparse, the general tendency of a lower abundance of refractory particles during PSC events compared to non-PSC situations was observed. The detection of such large refractory particles in the stratosphere, and the fact that these particles were not observed in the particle samples (upper size limit about 5 µm) taken during PSC events, strengthen the hypothesis that such particles are present in the polar stratosphere in late winter and that they can provide a surface for heterogeneous condensation during PSC formation.

scholarly journals HCl and ClO in activated Arctic air; first retrieved vertical profiles from TELIS submillimetre limb spectra

2012 ◽  
Vol 5 (2) ◽  
pp. 487-500 ◽  
Author(s):  
A. de Lange ◽  
M. Birk ◽  
G. de Lange ◽  
F. Friedl-Vallon ◽  
O. Kiselev ◽  
...  
Keyword(s):  
Michelson Interferometer ◽  
The Arctic ◽  
Optical Absorption Spectroscopy ◽  
Altitude Range ◽  
Balloon Flight ◽  
Total Uncertainty ◽  
Atmospheric Sounding ◽  
Systematic Effects ◽  
Equilibrium Profile ◽  
Peak Value

Abstract. The first profile retrieval results of the Terahertz and submillimeter Limb Sounder (TELIS) balloon instrument are presented. The spectra are recorded during a 13-h balloon flight on 24 January 2010 from Kiruna, Sweden. The TELIS instrument was mounted on the MIPAS-B2 gondola and shared this platform with the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) and the mini-Differential Optical Absorption Spectroscopy (mini-DOAS) instruments. The flight took place within the Arctic vortex at an altitude of ≈34 km in chlorine activated air, and both active (ClO) and inactive chlorine (HCl) were measured over an altitude range of respectively ≈16–32 km and ≈10–32 km. In this altitude range, the increase of ClO concentration levels during sunrise has been recorded with a temporal resolution of one minute. During the daytime equilibrium, a maximum ClO level of 2.1 ± 0.3 ppbv has been observed at an altitude of 23.5 km. This equilibrium profile is validated against the ClO profile by the satellite instrument Microwave Limb Sounder (MLS) aboard EOS Aura. HCl profiles have been determined from two different isotopes – H35Cl and H37Cl – and are also validated against MLS. The precision of all profiles is well below 0.01 ppbv and the overall accuracy is therefore governed by systematic effects. The total uncertainty of these effects is estimated to be maximal 0.3 ppbv for ClO around its peak value at 23.5 km during the daytime equilibrium, and for HCl it ranges from 0.05 to 0.4 ppbv, depending on altitude. In both cases the main uncertainty stems from a largely unknown non-linear response in the detector.

scholarly journals Chemical analysis of refractory stratospheric aerosol particles collected within the arctic vortex and inside polar stratospheric clouds

2016 ◽  
Vol 16 (13) ◽  
pp. 8405-8421 ◽  
Author(s):  
Martin Ebert ◽  
Ralf Weigel ◽  
Konrad Kandler ◽  
Gebhard Günther ◽  
Sergej Molleker ◽  
...  
Keyword(s):  
Aerosol Particles ◽  
Stratospheric Aerosol ◽  
The Arctic ◽  
Late Winter ◽  
General Tendency ◽  
Polar Stratospheric Clouds ◽  
Metal Mixtures ◽  
Air Masses ◽  
Size And Morphology ◽  
Stratospheric Clouds

Abstract. Stratospheric aerosol particles with diameters larger than about 10 nm were collected within the arctic vortex during two polar flight campaigns: RECONCILE in winter 2010 and ESSenCe in winter 2011. Impactors were installed on board the aircraft M-55 Geophysica, which was operated from Kiruna, Sweden. Flights were performed at a height of up to 21 km and some of the particle samples were taken within distinct polar stratospheric clouds (PSCs). The chemical composition, size and morphology of refractory particles were analyzed by scanning electron microscopy and energy-dispersive X-ray microanalysis. During ESSenCe no refractory particles with diameters above 500 nm were sampled. In total 116 small silicate, Fe-rich, Pb-rich and aluminum oxide spheres were found. In contrast to ESSenCe in early winter, during the late-winter RECONCILE mission the air masses were subsiding inside the Arctic winter vortex from the upper stratosphere and mesosphere, thus initializing a transport of refractory aerosol particles into the lower stratosphere. During RECONCILE, 759 refractory particles with diameters above 500 nm were found consisting of silicates, silicate ∕ carbon mixtures, Fe-rich particles, Ca-rich particles and complex metal mixtures. In the size range below 500 nm the presence of soot was also proven. While the data base is still sparse, the general tendency of a lower abundance of refractory particles during PSC events compared to non-PSC situations was observed. The detection of large refractory particles in the stratosphere, as well as the experimental finding that these particles were not observed in the particle samples (upper size limit ∼  5 µm) taken during PSC events, strengthens the hypothesis that such particles are present in the lower polar stratosphere in late winter and have provided a surface for heterogeneous nucleation during PSC formation.

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