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 ◽  
...  

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.

2011 ◽  
Vol 4 (5) ◽  
pp. 6497-6537 ◽  
Author(s):  
A. de Lange ◽  
M. Birk ◽  
G. de Lange ◽  
F. Friedl-Vallon ◽  
O. Kiselev ◽  
...  

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) have been 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 have been recorded with a temporal resolution of one minute. During the daytime equilibrium a maximum ClO level of 2.1 ± 0.3 ppb 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 ppb and the overall accuracy is therefore governed by systematic effects. The total uncertainty of these effects is estimated to be maximal 0.3 ppb 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 ppb depending on altitude. In both cases the main uncertainty stems from a largely unknown non-linear response in the detector.


2011 ◽  
Vol 11 (12) ◽  
pp. 33191-33227
Author(s):  
E. Arnone ◽  
E. Castelli ◽  
E. Papandrea ◽  
M. Carlotti ◽  
B. M. Dinelli

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.


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.


2014 ◽  
Vol 14 (7) ◽  
pp. 3247-3276 ◽  
Author(s):  
R. Hommel ◽  
K.-U. Eichmann ◽  
J. Aschmann ◽  
K. Bramstedt ◽  
M. Weber ◽  
...  

Abstract. Record breaking loss of ozone (O3) in the Arctic stratosphere has been reported in winter–spring 2010/2011. We examine in detail the composition and transformations occurring in the Arctic polar vortex using total column and vertical profile data products for O3, bromine oxide (BrO), nitrogen dioxide (NO2), chlorine dioxide (OClO), and polar stratospheric clouds (PSC) retrieved from measurements made by SCIAMACHY (Scanning Imaging Absorption SpectroMeter for Atmospheric CHartography) on-board Envisat (Environmental Satellite), as well as total column ozone amount, retrieved from the measurements of GOME-2 (Global Ozone Monitoring Experiment) on MetOp-A (Meteorological Experimental Satellite). Similarly we use the retrieved data from DOAS (Differential Optical Absorption Spectroscopy) measurements made in Ny-Ålesund (78.55° N, 11.55° E). A chemical transport model (CTM) has been used to relate and compare Arctic winter–spring conditions in 2011 with those in the previous year. In late winter–spring 2010/2011 the chemical ozone loss in the polar vortex derived from SCIAMACHY observations confirms findings reported elsewhere. More than 70% of O3 was depleted by halogen catalytic cycles between the 425 and 525 K isentropic surfaces, i.e. in the altitude range ~16–20 km. In contrast, during the same period in the previous winter 2009/2010, a typical warm Arctic winter, only slightly more than 20% depletion occurred below 20 km, while 40% of O3 was removed above the 575 K isentrope (~23 km). This loss above 575 K is explained by the catalytic destruction by NOx descending from the mesosphere. In both Arctic winters 2009/2010 and 2010/2011, calculated O3 losses from the CTM are in good agreement to our observations and other model studies. The mid-winter 2011 conditions, prior to the catalytic cycles being fully effective, are also investigated. Surprisingly, a significant loss of O3 around 60%, previously not discussed in detail, is observed in mid-January 2011 below 500 K (~19 km) and sustained for approximately 1 week. The low O3 region had an exceptionally large spatial extent. The situation was caused by two independently evolving tropopause elevations over the Asian continent. Induced adiabatic cooling of the stratosphere favoured the formation of PSC, increased the amount of active chlorine for a short time, and potentially contributed to higher polar ozone loss later in spring.


2021 ◽  
Author(s):  
Ramina Alwarda ◽  
Kristof Bognar ◽  
Kimberly Strong ◽  
Martyn Chipperfield ◽  
Sandip Dhomse ◽  
...  

<p>The Arctic winter of 2019-2020 was characterized by an unusually persistent polar vortex and temperatures in the lower stratosphere that were consistently below the threshold for the formation of polar stratospheric clouds (PSCs). These conditions led to ozone loss that is comparable to the Antarctic ozone hole. Ground-based measurements from a suite of instruments at the Polar Environment Atmospheric Research Laboratory (PEARL) in Eureka, Canada (80.05°N, 86.42°W) were used to investigate chemical ozone depletion. The vortex was located above Eureka longer than in any previous year in the 20-year dataset and lidar measurements provided evidence of polar stratospheric clouds (PSCs) above Eureka. Additionally, UV-visible zenith-sky Differential Optical Absorption Spectroscopy (DOAS) measurements showed record ozone loss in the 20-year dataset, evidence of denitrification along with the slowest increase of NO<sub>2</sub> during spring, as well as enhanced reactive halogen species (OClO and BrO). Complementary measurements of HCl and ClONO<sub>2</sub> (chlorine reservoir species) from a Fourier transform infrared (FTIR) spectrometer showed unusually low columns that were comparable to 2011, the previous year with significant chemical ozone depletion. Record low values of HNO<sub>3</sub> in the FTIR dataset are in accordance with the evidence of PSCs and a denitrified atmosphere. Estimates of chemical ozone loss were derived using passive ozone from the SLIMCAT offline chemical transport model to account for dynamical contributions to the stratospheric ozone budget.</p>


2012 ◽  
Vol 12 (15) ◽  
pp. 7073-7085 ◽  
Author(s):  
J. Kuttippurath ◽  
S. Godin-Beekmann ◽  
F. Lefèvre ◽  
G. Nikulin ◽  
M. L. Santee ◽  
...  

Abstract. We present a detailed discussion of the chemical and dynamical processes in the Arctic winters 1996/1997 and 2010/2011 with high resolution chemical transport model (CTM) simulations and space-based observations. In the Arctic winter 2010/2011, the lower stratospheric minimum temperatures were below 195 K for a record period of time, from December to mid-April, and a strong and stable vortex was present during that period. Simulations with the Mimosa-Chim CTM show that the chemical ozone loss started in early January and progressed slowly to 1 ppmv (parts per million by volume) by late February. The loss intensified by early March and reached a record maximum of ~2.4 ppmv in the late March–early April period over a broad altitude range of 450–550 K. This coincides with elevated ozone loss rates of 2–4 ppbv sh−1 (parts per billion by volume/sunlit hour) and a contribution of about 30–55% and 30–35% from the ClO-ClO and ClO-BrO cycles, respectively, in late February and March. In addition, a contribution of 30–50% from the HOx cycle is also estimated in April. We also estimate a loss of about 0.7–1.2 ppmv contributed (75%) by the NOx cycle at 550–700 K. The ozone loss estimated in the partial column range of 350–550 K exhibits a record value of ~148 DU (Dobson Unit). This is the largest ozone loss ever estimated in the Arctic and is consistent with the remarkable chlorine activation and strong denitrification (40–50%) during the winter, as the modeled ClO shows ~1.8 ppbv in early January and ~1 ppbv in March at 450–550 K. These model results are in excellent agreement with those found from the Aura Microwave Limb Sounder observations. Our analyses also show that the ozone loss in 2010/2011 is close to that found in some Antarctic winters, for the first time in the observed history. Though the winter 1996/1997 was also very cold in March–April, the temperatures were higher in December–February, and, therefore, chlorine activation was moderate and ozone loss was average with about 1.2 ppmv at 475–550 K or 42 DU at 350–550 K, as diagnosed from the model simulations and measurements.


2007 ◽  
Vol 7 (13) ◽  
pp. 3519-3536 ◽  
Author(s):  
A. Gobiet ◽  
G. Kirchengast ◽  
G. L. Manney ◽  
M. Borsche ◽  
C. Retscher ◽  
...  

Abstract. This study describes and evaluates a Global Navigation Satellite System (GNSS) radio occultation (RO) retrieval scheme particularly aimed at delivering bias-free atmospheric parameters for climate monitoring and research. The focus of the retrieval is on the sensible use of a priori information for careful high-altitude initialisation in order to maximise the usable altitude range. The RO retrieval scheme has been meanwhile applied to more than five years of data (September 2001 to present) from the German CHAllenging Minisatellite Payload for geoscientific research (CHAMP) satellite. In this study it was validated against various correlative datasets including the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) and the Global Ozone Monitoring for Occultation of Stars (GOMOS) sensors on Envisat, five different atmospheric analyses, and the operational CHAMP retrieval product from GeoForschungsZentrum (GFZ) Potsdam. In the global mean within 10 to 30 km altitude we find that the present validation observationally constrains the potential RO temperature bias to be <0.2 K. Latitudinally resolved analyses show biases to be observationally constrained to <0.2–0.5 K up to 35 km in most cases, and up to 30 km in any case, even if severely biased (about 10 K or more) a priori information is used in the high altitude initialisation of the retrieval. No evidence is found for the 10–35 km altitude range of residual RO bias sources other than those potentially propagated downward from initialisation, indicating that the widely quoted RO promise of "unbiasedness and long-term stability due to intrinsic self-calibration" can indeed be realised given care in the data processing to strictly limit structural uncertainty. The results thus reinforce that adequate high-altitude initialisation is crucial for accurate stratospheric RO retrievals. The common method of initialising, at some altitude in the upper stratosphere, the hydrostatic integral with an upper boundary temperature or pressure value derived from meteorological analyses is prone to introduce biases from the upper boundary down to below 25 km. Also above 30 to 35 km, GNSS RO delivers a considerable amount of observed information up to around 40 km, which is particularly interesting for numerical weather prediction (NWP) systems, where direct assimilation of non-initialised observed RO bending angles (free of a priori) is thus the method of choice. The results underline the value of RO for climate applications.


2005 ◽  
Vol 5 (3) ◽  
pp. 679-692 ◽  
Author(s):  
R. Spang ◽  
J. J. Remedios ◽  
L. J. Kramer ◽  
L. R. Poole ◽  
M. D. Fromm ◽  
...  

Abstract. The Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on ENVISAT has made extensive measurements of polar stratospheric clouds (PSCs) in the northern hemisphere winter 2002/2003. A PSC detection method based on a ratio of radiances (the cloud index) has been implemented for MIPAS and is validated in this study with respect to ground-based lidar and space borne occultation measurements. A very good correspondence in PSC sighting and cloud altitude between MIPAS detections and those of other instruments is found for cloud index values of less than four. Comparisons with data from the Stratospheric Aerosol and Gas Experiment (SAGE) III are used to further show that the sensitivity of the MIPAS detection method for this threshold value of cloud index is approximately equivalent to an extinction limit of 10-3km-1 at 1022nm, a wavelength used by solar occultation experiments. The MIPAS cloud index data are subsequently used to examine, for the first time with any technique, the evolution of PSCs throughout the Arctic polar vortex up to a latitude close to 90° north on a near-daily basis. We find that the winter of 2002/2003 is characterised by three phases of very different PSC activity. First, an unusual, extremely cold phase in the first three weeks of December resulted in high PSC occurrence rates. This was followed by a second phase of only moderate PSC activity from 5-13 January, separated from the first phase by a minor warming event. Finally there was a third phase from February to the end of March where only sporadic and mostly weak PSC events took place. The composition of PSCs during the winter period has also been examined, exploiting in particular an infra-red spectral signature which is probably characteristic of NAT. The MIPAS observations show the presence of these particles on a number of occasions in December but very rarely in January. The PSC type differentiation from MIPAS indicates that future comparisons of PSC observations with microphysical and denitrification models might be revealing about aspects of solid particle existence and location.


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