scholarly journals The Michelson Interferometer for Passive Atmospheric Sounding global climatology of BrONO<sub>2</sub> 2002–2012: a test for stratospheric bromine chemistry

2021 ◽  
Vol 21 (24) ◽  
pp. 18433-18464
Author(s):  
Michael Höpfner ◽  
Oliver Kirner ◽  
Gerald Wetzel ◽  
Björn-Martin Sinnhuber ◽  
Florian Haenel ◽  
...  

Abstract. We present the first observational dataset of vertically resolved global stratospheric BrONO2 distributions from July 2002 until April 2012 and compare them to results of the atmospheric chemical climate model ECHAM/MESSy Atmospheric Chemistry (EMAC). The retrieved distributions are based on space-borne measurements of infrared limb-emission spectra recorded by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on Envisat. The derived vertical profiles of BrONO2 volume mixing ratios represent 10∘ latitude bins and 3 d means, separated into sunlit observations and observations in the dark. The estimated uncertainties are around 1–4 pptv, caused by spectral noise for single profiles as well as for further parameter and systematic errors which may not improve by averaging. Vertical resolutions range from 3 to 8 km between 15 and 35 km altitude. All leading modes of spatial and temporal variability of stratospheric BrONO2 in the observations are well replicated by the model simulations: the large diurnal variability, the low values during polar winter as well as the maximum values at mid and high latitudes during summer. Three major differences between observations and model results are observed: (1) a model underestimation of enhanced BrONO2 in the polar winter stratosphere above about 30 km of up to 15 pptv, (2) up to 8 pptv higher modelled values than observed globally in the lower stratosphere up to 25 km, most obvious during night, and (3) up to 5 pptv lower modelled concentrations at tropical latitudes between 27 and 32 km during sunlit conditions. (1) is explained by the model missing enhanced NOx produced in the mesosphere and lower thermosphere subsiding at high latitudes in winter. This is the first time that observational evidence for enhancement of BrONO2 caused by mesospheric NOx production is reported. The other major inconsistencies (2, 3) between EMAC model results and observations are studied by sensitivity runs with a 1D model. These tentatively hint at a model underestimation of heterogeneous loss of BrONO2 in the lower stratosphere, a simulated production of BrONO2 that is too low during the day as well as strongly underestimated BrONO2 volume mixing ratios when loss via reaction with O(3P) is considered in addition to photolysis. However, considering the uncertainty ranges of model parameters and of measurements, an unambiguous identification of the causes of the differences remains difficult. The observations have also been used to derive the total stratospheric bromine content relative to years of stratospheric entry between 1997 and 2007. With an average value of 21.2±1.4 pptv of Bry at mid latitudes where the modelled adjustment from BrONO2 to Bry is smallest, the MIPAS data agree with estimates of Bry derived from observations of BrO as well as from MIPAS-Balloon measurements of BrONO2.

2021 ◽  
Author(s):  
Michael Höpfner ◽  
Oliver Kirner ◽  
Gerald Wetzel ◽  
Björn-Martin Sinnhuber ◽  
Florian Haenel ◽  
...  

Abstract. We present the first observational dataset of vertically resolved global stratospheric BrONO2 distributions from July 2002 until April 2012, and compare them to results of the atmospheric chemical climate model EMAC. The retrieved distributions are based on space-borne measurements of infrared limb-emission spectra recorded by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on Envisat. The derived vertical profiles of BrONO2 volume mixing ratios represent 10° latitude bins and three-day means, separated into sunlit and observations in the dark. The estimated uncertainties are around 1–4 pptv caused by spectral noise for single profiles as well as for further parameter and systematic errors which may not improve by averaging. Vertical resolutions range from 3 to 8 km between 15 and 35 km altitude. All leading modes of spatial and temporal variability of stratospheric BrONO2 in the observations are well replicated by the model simulations: the large diurnal variability, the low values during polar winter as well as the maximum values at mid- and high latitudes during summer. Three major differences between observations and model results are observed: (1) a model underestimation of enhanced BrONO2 in the polar winter stratosphere above about 30 km of up to 15 pptv, (2) up to 8 pptv higher modelled values than observed globally in the lower stratosphere up to 25 km most obvious during night, and (3) up to 5 pptv lower modelled concentrations at tropical latitudes between 27 and 32 km during sunlit conditions. (1) is explained by the model missing enhanced NOx produced in the mesosphere and lower thermosphere subsiding at high latitudes in winter. This is the first time that observational evidence for enhancement of BrONO2 caused by mesospheric NOx production is reported. The other major inconsistencies (2,3) between EMAC model results and observations are studied by sensitivity runs with a 1d model. These tentatively hint to a model underestimation of heterogeneous loss of BrONO2 in the lower stratosphere, a too low simulated production of BrONO2 during day as well as strongly underestimated BrONO2 volume mixing ratios when loss via reaction with O(3P) is considered additionally to photolysis. However, considering the uncertainty ranges of model parameters and of measurements, an unambiguous identification of the causes for the differences remains difficult. The observations have also been used to derive the total stratospheric bromine content relative to years of stratospheric entry between 1997 and 2007. With an average value of 21.2 ± 1.4 pptv of Bry at mid-latitudes where the modelled adjustment from BrONO2 to Bry is lowest, the MIPAS data agree with estimates of Bry derived from observations of BrO as well as from MIPAS-Balloon measurements of BrONO2.


2007 ◽  
Vol 7 (4) ◽  
pp. 10515-10541
Author(s):  
D. P. Moore ◽  
J. J. Remedios

Abstract. The Michelson Interferometer for Passive Atmospheric Sounding onboard ENVISAT (MIPAS-E) offers the opportunity to detect and spectrally resolve many atmospheric minor constituents affecting atmospheric chemistry. In this paper, we describe an algorithm produced to retrieve HCFC–22 profiles from MIPAS-E measurements made in 2003 and present results from this scheme between 300 and 50 mb. By comparison with ATMOS (AT–3) version 3 data, we find a mean Northern Hemisphere mid-latitude (20–50° N) HCFC–22 growth rate between 1994 and 2003 of 5.4±0.7 pptv/yr in the lower stratosphere (LS) and a mean LS Southern Hemisphere growth rate (60–80°S) of 6.0±0.7 pptv/yr in the same period. We test the feasibility of using a global data set to estimate the chemical lifetime of HCFC–22 in the LS and we derive this for two regions; 20–50° N (259±38 years) and 60–80° S (288±34 years). From these data we note a global LS lifetime of 274±25 years, significantly longer than previous estimates.


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.


2008 ◽  
Vol 8 (1) ◽  
pp. 73-82 ◽  
Author(s):  
D. P. Moore ◽  
J. J. Remedios

Abstract. The Michelson Interferometer for Passive Atmospheric Sounding onboard ENVISAT (MIPAS-E) offers the opportunity to detect and spectrally resolve many atmospheric minor constituents affecting atmospheric chemistry. In this paper, we describe an algorithm produced to retrieve HCFC–22 profiles from MIPAS-E measurements made in 2003 and present results from this scheme between 300 and 50 mb. By comparison with ATMOS (AT–3) version 3 data, we find a mean Northern Hemisphere mid-latitude (20–50° N) HCFC–22 growth rate between 1994 and 2003 of 5.4±0.7 pptv/yr in the lower stratosphere (LS) and a mean LS Southern Hemisphere growth rate (60–80° S) of 6.0±0.7 pptv/yr in the same period. We test the feasibility of using a global data set to estimate the chemical lifetime of HCFC–22 in the LS and we derive this for two regions: 20–50° N (246±38 years) and 60–80° S (274±34 years). From these data we note a global LS lifetime of 260±25 years, significantly longer than previous estimates.


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.


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.


2017 ◽  
Vol 17 (18) ◽  
pp. 11521-11539 ◽  
Author(s):  
Stefan Lossow ◽  
Hella Garny ◽  
Patrick Jöckel

Abstract. The amplitude of the annual variation in water vapour exhibits a distinct isolated maximum in the middle and upper stratosphere in the southern tropics and subtropics, peaking typically around 15° S in latitude and close to 3 hPa (∼  40.5 km) in altitude. This enhanced annual variation is primarily related to the Brewer–Dobson circulation and hence also visible in other trace gases. So far this feature has not gained much attention in the literature and the present work aims to add more prominence. Using Envisat/MIPAS (Environmental Satellite/Michelson Interferometer for Passive Atmospheric Sounding) observations and ECHAM/MESSy (European Centre for Medium-Range Weather Forecasts Hamburg/Modular Earth Submodel System) Atmospheric Chemistry (EMAC) simulations we provide a dedicated illustration and a full account of the reasons for this enhanced annual variation.


2015 ◽  
Vol 8 (12) ◽  
pp. 5251-5261 ◽  
Author(s):  
A. Laeng ◽  
J. Plieninger ◽  
T. von Clarmann ◽  
U. Grabowski ◽  
G. Stiller ◽  
...  

Abstract. The Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) is an infrared (IR) limb emission spectrometer on the Envisat platform. It measures trace gas distributions during day and night, pole-to-pole, over an altitude range from 6 to 70 km in nominal mode and up to 170 km in special modes, depending on the measurement mode, producing more than 1000 profiles day−1. We present the results of a validation study of methane, version V5R_CH4_222, retrieved with the IMK/IAA (Institut für Meteorologie und Klimaforschung, Karlsruhe/Instituto de Astrofisica de Andalucia, Grenada) MIPAS scientific level 2 processor. The level 1 spectra are provided by the ESA (European Space Agency) and version 5 was used. The time period covered is 2005–2012, which corresponds to the period when MIPAS measured trace gas distributions at a reduced spectral resolution of 0.0625 cm−1. The comparison with satellite instruments includes the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS), the HALogen Occultation Experiment (HALOE), the Solar Occultation For Ice Experiment (SOFIE) and the SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY). Furthermore, comparisons with MkIV balloon-borne solar occultation measurements and with air sampling measurements performed by the University of Frankfurt are presented. The validation activities include bias determination, assessment of stability, precision validation, analysis of histograms and comparison of corresponding climatologies. Above 50 km altitude, MIPAS methane mixing ratios agree within 3 % with ACE-FTS and SOFIE. Between 30 and 40 km an agreement within 3 % with SCIAMACHY has been found. In the middle stratosphere, there is no clear indication of a MIPAS bias since comparisons with various instruments contradict each other. In the lower stratosphere (below 25 km) MIPAS CH4 is biased high with respect to satellite instruments, and the most likely estimate of this bias is 14 %. However, in the comparison with CH4 data obtained from cryogenic whole-air sampler (cryosampler) measurements, there is no evidence of a high bias in MIPAS between 20 and 25 km altitude. Precision validation is performed on collocated MIPAS–MIPAS pairs and suggests a slight underestimation of its uncertainties by a factor of 1.2. No significant evidence of an instrumental drift has been found.


2015 ◽  
Vol 15 (16) ◽  
pp. 22291-22329 ◽  
Author(s):  
C. E. Sioris ◽  
J. Zou ◽  
D. A. Plummer ◽  
C. D. Boone ◽  
C. T. McElroy ◽  
...  

Abstract. Seasonal and monthly zonal medians of water vapour in the upper troposphere and lower stratosphere (UTLS) are calculated for both Atmospheric Chemistry Experiment (ACE) instruments for the northern and southern high-latitude regions (60–90 and 60–90° S). Chosen for the purpose of observing high-latitude processes, the ACE orbit provides sampling of both regions in eight of 12 months of the year, with coverage in all seasons. The ACE water vapour sensors, namely MAESTRO (Measurements of Aerosol Extinction in the Stratosphere and Troposphere Retrieved by Occultation) and the Fourier Transform Spectrometer (ACE-FTS) are currently the only satellite instruments that can probe from the lower stratosphere down to the mid-troposphere to study the vertical profile of the response of UTLS water vapour to the annular modes. The Arctic oscillation (AO), also known as the northern annular mode (NAM), explains 64 % (r = −0.80) of the monthly variability in water vapour at northern high-latitudes observed by ACE-MAESTRO between 5 and 7 km using only winter months (January to March 2004–2013). Using a seasonal timestep and all seasons, 45 % of the variability is explained by the AO at 6.5 ± 0.5 km, similar to the 46 % value obtained for southern high latitudes at 7.5 ± 0.5 km explained by the Antarctic oscillation or southern annular mode (SAM). A large negative AO event in March 2013 produced the largest relative water vapour anomaly at 5.5 km (+70 %) over the ACE record. A similarly large event in the 2010 boreal winter, which was the largest negative AO event in the record (1950–2015), led to > 50 % increases in water vapour observed by MAESTRO and ACE-FTS at 7.5 km.


2020 ◽  
Vol 13 (1) ◽  
pp. 287-308
Author(s):  
Stefan Lossow ◽  
Charlotta Högberg ◽  
Farahnaz Khosrawi ◽  
Gabriele P. Stiller ◽  
Ralf Bauer ◽  
...  

Abstract. The annual variation of δD in the tropical lower stratosphere is a critical indicator for the relative importance of different processes contributing to the transport of water vapour through the cold tropical tropopause region into the stratosphere. Distinct observational discrepancies of the δD annual variation were visible in the works of Steinwagner et al. (2010) and Randel et al. (2012). Steinwagner et al. (2010) analysed MIPAS (Michelson Interferometer for Passive Atmospheric Sounding) observations retrieved with the IMK/IAA (Institut für Meteorologie und Klimaforschung in Karlsruhe, Germany, in collaboration with the Instituto de Astrofísica de Andalucía in Granada, Spain) processor, while Randel et al. (2012) focused on ACE-FTS (Atmospheric Chemistry Experiment Fourier Transform Spectrometer) observations. Here we reassess the discrepancies based on newer MIPAS (IMK/IAA) and ACE-FTS data sets, also showing for completeness results from SMR (Sub-Millimetre Radiometer) observations and a ECHAM/MESSy (European Centre for Medium-Range Weather Forecasts Hamburg and Modular Earth Submodel System) Atmospheric Chemistry (EMAC) simulation (Eichinger et al., 2015b). Similar to the old analyses, the MIPAS data set yields a pronounced annual variation (maximum about 75 ‰), while that derived from the ACE-FTS data set is rather weak (maximum about 25 ‰). While all data sets exhibit the phase progression typical for the tape recorder, the annual maximum in the ACE-FTS data set precedes that in the MIPAS data set by 2 to 3 months. We critically consider several possible reasons for the observed discrepancies, focusing primarily on the MIPAS data set. We show that the δD annual variation in the MIPAS data up to an altitude of 40 hPa is substantially impacted by a “start altitude effect”, i.e. dependency between the lowermost altitude where MIPAS retrievals are possible and retrieved data at higher altitudes. In itself this effect does not explain the differences with the ACE-FTS data. In addition, there is a mismatch in the vertical resolution of the MIPAS HDO and H2O data (being consistently better for HDO), which actually results in an artificial tape-recorder-like signal in δD. Considering these MIPAS characteristics largely removes any discrepancies between the MIPAS and ACE-FTS data sets and shows that the MIPAS data are consistent with a δD tape recorder signal with an amplitude of about 25 ‰ in the lowermost stratosphere.


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