scholarly journals Sulfur dioxide (SO<sub>2</sub>) from MIPAS in the upper troposphere and lower stratosphere 2002–2012

2015 ◽  
Vol 15 (12) ◽  
pp. 7017-7037 ◽  
Author(s):  
M. Höpfner ◽  
C. D. Boone ◽  
B. Funke ◽  
N. Glatthor ◽  
U. Grabowski ◽  
...  

Abstract. Vertically resolved distributions of sulfur dioxide (SO2) with global coverage in the height region from the upper troposphere to ~20 km altitude have been derived from observations by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on Envisat for the period July 2002 to April 2012. Retrieved volume mixing ratio profiles representing single measurements are characterized by typical errors in the range of 70–100 pptv and by a vertical resolution ranging from 3 to 5 km. Comparison with observations by the Atmospheric Chemistry Experiment Fourier transform spectrometer (ACE-FTS) revealed a slightly varying bias with altitude of −20 to 50 pptv for the MIPAS data set in case of volcanically enhanced concentrations. For background concentrations the comparison showed a systematic difference between the two major MIPAS observation periods. After debiasing, the difference could be reduced to biases within −10 to 20 pptv in the altitude range of 10–20 km with respect to ACE-FTS. Further comparisons of the debiased MIPAS data set with in situ measurements from various aircraft campaigns showed no obvious inconsistencies within a range of around ±50 pptv. The SO2 emissions of more than 30 volcanic eruptions could be identified in the upper troposphere and lower stratosphere (UTLS). Emitted SO2 masses and lifetimes within different altitude ranges in the UTLS have been derived for a large part of these eruptions. Masses are in most cases within estimations derived from other instruments. From three of the major eruptions within the MIPAS measurement period – Kasatochi in August 2008, Sarychev in June 2009 and Nabro in June 2011 – derived lifetimes of SO2 for the altitude ranges 10–14, 14–18 and 18–22 km are 13.3 ± 2.1, 23.6 ± 1.2 and 32.3 ± 5.5 days respectively. By omitting periods with obvious volcanic influence we have derived background mixing ratio distributions of SO2. At 10 km altitude these indicate an annual cycle at northern mid- and high latitudes with maximum values in summer and an amplitude of about 30 pptv. At higher altitudes of about 16–18 km, enhanced mixing ratios of SO2 can be found in the regions of the Asian and the North American monsoons in summer – a possible connection to an aerosol layer discovered by Vernier et al. (2011b) in that region.

2015 ◽  
Vol 15 (4) ◽  
pp. 5801-5847 ◽  
Author(s):  
M. Höpfner ◽  
C. D. Boone ◽  
B. Funke ◽  
N. Glatthor ◽  
U. Grabowski ◽  
...  

Abstract. Vertically resolved distributions of sulfur dioxide (SO2) with global coverage in the height region from the upper troposphere to ~ 20 km altitude have been derived from observations by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on Envisat for the period July 2002 to April 2012. Retrieved volume mixing ratio profiles representing single measurements are characterized by typical errors in the range of 70–100 pptv and by a vertical resolution ranging from 3–5 km. Comparison with ACE-FTS observations revealed a slightly varying bias with altitude of −20 to 50 pptv for the MIPAS dataset in case of volcanically enhanced concentrations. For background concentrations the comparison showed a systematic difference between the two major MIPAS observation periods. After debiasing, the difference could be reduced to biases within −10 to 20 pptv in the altitude range of 10–20 km with respect to ACE-FTS. Further comparisons of the debiased MIPAS dataset with in-situ measurements from various aircraft campaigns showed no obvious inconsistencies within a range of around ±50 pptv. The SO2 emissions of more than thirty volcanic eruptions could be identified in the upper troposphere and lower stratosphere (UTLS). Emitted SO2 masses and lifetimes within different altitude ranges in the UTLS have been derived for a large part of these eruptions. Masses are in most cases within estimations derived from other instruments. From three of the major eruptions within the MIPAS measurement period – Kasatochi in August 2008, Sarychev in June 2009 and Nabro in June 2011 – derived lifetimes of SO2 for the altitude ranges 10–14, 14–18, and 18–22 km are 13.3±2.1, 23.6±1.2, and 32.3±5.5 d, respectively. By omitting periods with obvious volcanic influence we have derived background mixing ratio distributions of SO2. At 10 km altitude these indicate an annual cycle at northern mid- and high latitudes with maximum values in summer and an amplitude of about 30 pptv. At higher altitudes of about 16–18 km enhanced mixing ratios of SO2 can be found in the region of the Asian and the North-American monsoon in summer – a possible connection to an aerosol layer discovered by Vernier et al. (2011b) in that region.


2015 ◽  
Vol 8 (1) ◽  
pp. 195-209 ◽  
Author(s):  
H. C. Pumphrey ◽  
W. G. Read ◽  
N. J. Livesey ◽  
K. Yang

Abstract. Sulfur dioxide (SO2) is an important atmospheric constituent, particularly in the aftermath of volcanic eruptions. These events can inject large amounts of SO2 into the lower stratosphere, where it is oxidised to form sulfate aerosols; these in turn have a significant effect on the climate. The MLS instrument on the Aura satellite has observed the SO2 mixing ratio in the upper troposphere and lower stratosphere from August 2004 to the present, during which time a number of volcanic eruptions have significantly affected those regions of the atmosphere. We describe the MLS SO2 data and how various volcanic events appear in the data. As the MLS SO2 data are currently not validated we take some initial steps towards their validation. First we establish the level of internal consistency between the three spectral regions in which MLS is sensitive to SO2. We compare SO2 column values calculated from MLS data to total column values reported by the OMI instrument. The agreement is good (within about 1 DU) in cases where the SO2 is clearly at altitudes above 147 hPa.


2019 ◽  
Vol 19 (4) ◽  
pp. 2497-2526 ◽  
Author(s):  
Charlotta Högberg ◽  
Stefan Lossow ◽  
Farahnaz Khosrawi ◽  
Ralf Bauer ◽  
Kaley A. Walker ◽  
...  

Abstract. Within the framework of the second SPARC (Stratosphere-troposphere Processes And their Role in Climate) water vapour assessment (WAVAS-II), we evaluated five data sets of δD(H2O) obtained from observations by Odin/SMR (Sub-Millimetre Radiometer), Envisat/MIPAS (Environmental Satellite/Michelson Interferometer for Passive Atmospheric Sounding), and SCISAT/ACE-FTS (Science Satellite/Atmospheric Chemistry Experiment – Fourier Transform Spectrometer) using profile-to-profile and climatological comparisons. These comparisons aimed to provide a comprehensive overview of typical uncertainties in the observational database that could be considered in the future in observational and modelling studies. Our primary focus is on stratospheric altitudes, but results for the upper troposphere and lower mesosphere are also shown. There are clear quantitative differences in the measurements of the isotopic ratio, mainly with regard to comparisons between the SMR data set and both the MIPAS and ACE-FTS data sets. In the lower stratosphere, the SMR data set shows a higher depletion in δD than the MIPAS and ACE-FTS data sets. The differences maximise close to 50 hPa and exceed 200 ‰. With increasing altitude, the biases decrease. Above 4 hPa, the SMR data set shows a lower δD depletion than the MIPAS data sets, occasionally exceeding 100 ‰. Overall, the δD biases of the SMR data set are driven by HDO biases in the lower stratosphere and by H2O biases in the upper stratosphere and lower mesosphere. In between, in the middle stratosphere, the biases in δD are the result of deviations in both HDO and H2O. These biases are attributed to issues with the calibration, in particular in terms of the sideband filtering, and uncertainties in spectroscopic parameters. The MIPAS and ACE-FTS data sets agree rather well between about 100 and 10 hPa. The MIPAS data sets show less depletion below approximately 15 hPa (up to about 30 ‰), due to differences in both HDO and H2O. Higher up this behaviour is reversed, and towards the upper stratosphere the biases increase. This is driven by increasing biases in H2O, and on occasion the differences in δD exceed 80 ‰. Below 100 hPa, the differences between the MIPAS and ACE-FTS data sets are even larger. In the climatological comparisons, the MIPAS data sets continue to show less depletion in δD than the ACE-FTS data sets below 15 hPa during all seasons, with some variations in magnitude. The differences between the MIPAS and ACE-FTS data have multiple causes, such as differences in the temporal and spatial sampling (except for the profile-to-profile comparisons), cloud influence, vertical resolution, and the microwindows and spectroscopic database chosen. Differences between data sets from the same instrument are typically small in the stratosphere. Overall, if the data sets are considered together, the differences in δD among them in key areas of scientific interest (e.g. tropical and polar lower stratosphere, lower mesosphere, and upper troposphere) are too large to draw robust conclusions on atmospheric processes affecting the water vapour budget and distribution, e.g. the relative importance of different mechanisms transporting water vapour into the stratosphere.


2016 ◽  
Vol 9 (9) ◽  
pp. 4355-4373 ◽  
Author(s):  
Swagata Payra ◽  
Philippe Ricaud ◽  
Rachid Abida ◽  
Laaziz El Amraoui ◽  
Jean-Luc Attié ◽  
...  

Abstract. The present analysis deals with one of the most debated aspects of the studies on the upper troposphere/lower stratosphere (UTLS), namely the budget of water vapour (H2O) at the tropical tropopause. Within the French project “Multiscale water budget in the upper troposphere and lower stratosphere in the TROpics” (TRO-pico), a global-scale analysis has been set up based on space-borne observations, models and assimilation techniques. The MOCAGE-VALENTINA assimilation tool has been used to assimilate the Aura Microwave Limb Sounder (MLS) version 3.3 H2O measurements within the 316–5 hPa range from August 2011 to March 2013 with an assimilation window of 1 h. Diagnostics based on observations minus analysis and forecast are developed to assess the quality of the assimilated H2O fields. Comparison with an independent source of H2O measurements in the UTLS based on the space-borne Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) observations and with meteorological ARPEGE analyses is also shown. Sensitivity studies of the analysed fields have been performed by (1) considering periods when no MLS measurements are available and (2) using H2O data from another MLS version (4.2). The studies have been performed within three different spaces in time and space coincidences with MLS (hereafter referred to as MLS space) and MIPAS (MIPAS space) observations and with the model (model space) outputs and at three different levels: 121 hPa (upper troposphere), 100 hPa (tropopause) and 68 hPa (lower stratosphere) in January and February 2012. In the MLS space, the analyses behave consistently with the MLS observations from the upper troposphere to the lower stratosphere. In the model space, the analyses are wetter than the reference atmosphere as represented by ARPEGE and MLS in the upper troposphere (121 hPa) and around the tropopause (100 hPa), but are consistent with MLS and MIPAS in the lower stratosphere (68 hPa). In the MIPAS space, the sensitivity and the vertical resolution of the MIPAS data set at 121 and 100 hPa prevent assessment of the behaviour of the analyses at 121 and 100 hPa, particularly over intense convective areas as the South American, the African and the Maritime continents but, in the lower stratosphere (68 hPa), the analyses are very consistent with MIPAS. Sensitivity studies show the improvement on the H2O analyses in the tropical UTLS when assimilating space-borne measurements of better quality, particularly over the convective areas.


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.


2018 ◽  
Author(s):  
Charlotta Högberg ◽  
Stefan Lossow ◽  
Ralf Bauer ◽  
Kaley A. Walker ◽  
Patrick Eriksson ◽  
...  

Abstract. Within the framework of the second SPARC (Stratosphere-troposphere Processes And their Role in Climate) water vapour assessment (WAVAS-II), we have evaluated five data sets of δD(H2O) obtained from observations of Odin/SMR (Sub-Millimetre Radiometer), Envisat/MIPAS (Environmental Satellite/Michelson Interferometer for Passive Atmospheric Sounding) and SCISAT/ACE-FTS (Science Satellite/Atmospheric Chemistry Experiment-Fourier Transform Spectrometer) using profile-to-profile and climatological comparisons. Our focus is on stratospheric altitudes, but results from the upper troposphere to the lower mesosphere are provided. There are clear quantitative differences in the measurements of the isotopic ratio, which primarily concerns the comparisons to the SMR data set. In the lower stratosphere, this data set shows a higher depletion than the MIPAS and ACE-FTS data sets. The differences maximise close to 50 hPa and exceed 200 per mille. With increasing altitude, the biases typically decrease. Above 4 hPa, the SMR data set shows a lower depletion than the MIPAS data sets, on occasion exceeding 100 per mille. Overall, the δD biases of the SMR data set are driven by HDO biases in the lower stratosphere and by H2O biases in the upper stratosphere and lower mesosphere. In between, in the middle stratosphere, the biases in δD are a combination of deviations in both HDO and H2O. These biases are attributed to issues with the calibration, in particular in terms of the sideband filtering for H2O, and uncertainties in spectroscopic parameters. The MIPAS and ACE-FTS data sets agree rather well between about 100 hPa and 10 hPa. The MIPAS data sets show less depletion below about 15 hPa (up to about 30 per mille), due to differences in both HDO and H2O. Higher up the picture is reversed, and towards the upper stratosphere the biases typically increase. This is driven by increasing biases in H2O and on occasion the differences in δD exceed 80 per mille. Below 100 hPa, the differences between the MIPAS and ACE-FTS data sets are even larger. In the climatological comparisons, the MIPAS data sets continue to show less depletion than the ACE-FTS data sets below 15 hPa during all seasons, with some variations in magnitude. The differences between the MIPAS and ACE-FTS data come from different aspects, such as differences in the temporal and spatial sampling (except for the profile-to-profile comparisons), cloud influence, vertical resolution, and the microwindows and spectroscopic database chosen. Differences between data sets from the same instrument are typically small in the stratosphere.


2020 ◽  
Author(s):  
Masatomo Fujiwara ◽  
Tetsu Sakai ◽  
Koichi Shiraishi ◽  
Yoichi Inai ◽  
Sergey Khaykin ◽  
...  

Abstract. Eastward airmass transport from the Asian summer monsoon (ASM) anticyclone in the upper troposphere and lower stratosphere (UTLS) often involves eastward shedding vortices, which can cover most of the Japanese archipelago. We investigated the aerosol characteristics of these vortices by analysing data from two lidar systems in Japan, at Tsukuba (36.1° N, 140.1° E) and Fukuoka (33.55° N, 130.36° E), during the summer of 2018. We observed several events with enhanced particle signals at Tsukuba at 15.5–18 km altitude (at or above the local tropopause) during August–September 2018, with a backscattering ratio of ~1.10 and particle depolarization of ~5 % (i.e., not spherical, but more spherical than ice crystals). These particle characteristics may be consistent with those of solid aerosol particles, such as ammonium nitrate. Each event had a timescale of a few days. During the same study period, we also observed similar enhanced particle signals in the lower stratosphere at Fukuoka. The upper troposphere is often covered by cirrus clouds at both lidar sites. Backward trajectory calculations for these sites for days with enhanced particle signals in the lower stratosphere and days without indicate that the former airmasses originated within the ASM anticyclone, and the latter more from edge regions. Reanalysis carbon-monoxide and satellite water-vapour data indicate that eastward shedding vortices were involved in the observed aerosol enhancements. Satellite aerosol data confirm that the period and latitudinal region were free from the direct influence of documented volcanic eruptions and high latitude forest fires. Our results indicate that the Asian Tropopause Aerosol Layer (ATAL) over the ASM region extends east towards Japan in association with the eastward shedding vortices, and that lidar systems in Japan can detect at least the lower stratospheric portion of the ATAL during periods when the lower stratosphere is undisturbed by volcanic eruptions and forest fires. The upper tropospheric portion of the ATAL is either depleted by tropospheric processes (convection and wet scavenging) during eastward transport or is obscured by much stronger cirrus cloud signals.


2021 ◽  
Vol 21 (4) ◽  
pp. 3073-3090
Author(s):  
Masatomo Fujiwara ◽  
Tetsu Sakai ◽  
Tomohiro Nagai ◽  
Koichi Shiraishi ◽  
Yoichi Inai ◽  
...  

Abstract. Eastward air-mass transport from the Asian summer monsoon (ASM) anticyclone in the upper troposphere and lower stratosphere (UTLS) often involves eastward-shedding vortices, which can cover most of the Japanese archipelago. We investigated the aerosol characteristics of these vortices by analysing data from two lidar systems in Japan, at Tsukuba (36.1∘ N, 140.1∘ E) and Fukuoka (33.55∘ N, 130.36∘ E), during the summer of 2018. We observed several events with enhanced particle signals at Tsukuba at 15.5–18 km of altitude (at or above the local tropopause) during August–September 2018, with a backscattering ratio of ∼ 1.10 and particle depolarization of ∼ 5 % (i.e. not spherical, but more spherical than ice crystals). These particle characteristics may be consistent with those of solid aerosol particles, such as ammonium nitrate. Each event had a timescale of a few days. During the same study period, we also observed similar enhanced particle signals in the lower stratosphere at Fukuoka. The upper troposphere is often covered by cirrus clouds at both lidar sites. Backward trajectory calculations for these sites for days with enhanced particle signals in the lower stratosphere and days without indicate that the former air masses originated within the ASM anticyclone and the latter more from edge regions. Reanalysis carbon monoxide and satellite water vapour data indicate that eastward-shedding vortices were involved in the observed aerosol enhancements. Satellite aerosol data confirm that the period and latitudinal region were free from the direct influence of documented volcanic eruptions and high-latitude forest fires. Our results indicate that the Asian tropopause aerosol layer (ATAL) over the ASM region extends east towards Japan in association with the eastward-shedding vortices and that lidar systems in Japan can detect at least the lower-stratospheric portion of the ATAL during periods when the lower stratosphere is undisturbed by volcanic eruptions and forest fires. The upper-tropospheric portion of the ATAL is either depleted by tropospheric processes (convection and wet scavenging) during eastward transport or is obscured by much stronger cirrus cloud signals.


2016 ◽  
Author(s):  
R. J. Pope ◽  
N. A. D. Richards ◽  
M. P. Chipperfield ◽  
D. P. Moore ◽  
S. A. Monks ◽  
...  

Abstract. Peroxyacetyl nitrate (PAN) is an important chemical species in the troposphere as it aids the long-range transport of NOx and subsequent formation of O3 in relatively clean remote regions. Over the past few decades observations from aircraft campaigns and surface sites have been used to better understand the regional distribution of PAN. However, recent measurements made by satellites allow for a global assessment of PAN in the upper troposphere – lower stratosphere (UTLS). In this study, we investigate global PAN distributions from two independent retrieval methodologies, based on measurements from the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) instrument, on board ENVISAT from the Institute of Meteorology and Climate Research (IMK), Karlsruhe Institute of Technology and the Department of Physics and Astronomy, University of Leicester (UoL). Retrieving PAN from MIPAS is challenging due to the weak signal in the measurements and contamination from other species. Therefore, we compare the two MIPAS datasets with observations from the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS), insitu aircraft data and the TOMCAT 3-D chemical transport model. MIPAS shows peak UTLS PAN concentrations over the biomass burning regions (e.g. ranging from 150 to > 200 pptv at 150 hPa) and during the summertime Asian monsoon as enhanced convection aids the vertical transport of PAN from the lower atmosphere. At 150 hPa, we find significant differences between the two MIPAS datasets in the tropics, where IMK PAN concentrations are larger by 50–100 pptv. Comparisons between MIPAS and ACE-FTS show better agreement with the UoL MIPAS PAN concentrations at 200 hPa, but with mixed results above this altitude. TOMCAT generally captures the magnitude and structure of climatological aircraft PAN profiles within the observational variability allowing it to be used to investigate the MIPAS PAN differences. TOMCAT-MIPAS comparisons show that the model is both positively (UoL) and negatively (IMK) biased against the satellite products. These results show that satellite PAN observations are able to detect realistic spatial variations in PAN in the UTLS, but further work is needed to resolve differences in existing retrievals to allow quantitative use of the products.


Science ◽  
2012 ◽  
Vol 337 (6090) ◽  
pp. 78-81 ◽  
Author(s):  
Adam E. Bourassa ◽  
Alan Robock ◽  
William J. Randel ◽  
Terry Deshler ◽  
Landon A. Rieger ◽  
...  

The Nabro stratovolcano in Eritrea, northeastern Africa, erupted on 13 June 2011, injecting approximately 1.3 teragrams of sulfur dioxide (SO2) to altitudes of 9 to 14 kilometers in the upper troposphere, which resulted in a large aerosol enhancement in the stratosphere. The SO2 was lofted into the lower stratosphere by deep convection and the circulation associated with the Asian summer monsoon while gradually converting to sulfate aerosol. This demonstrates that to affect climate, volcanic eruptions need not be strong enough to inject sulfur directly to the stratosphere.


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