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

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 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 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.


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.


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.


2014 ◽  
Vol 7 (7) ◽  
pp. 7883-7922
Author(s):  
H. C. Pumphrey ◽  
W. G. Read ◽  
N. J. Livesey ◽  
K. Yang

Abstract. Sulphur 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 sulphate 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 in cases where the SO2 is clearly at altitudes above 147 hPa.


2016 ◽  
Vol 9 (2) ◽  
pp. 793-815 ◽  
Author(s):  
Kai-Uwe Eichmann ◽  
Luca Lelli ◽  
Christian von Savigny ◽  
Harjinder Sembhi ◽  
John P. Burrows

Abstract. Cloud top heights (CTHs) are retrieved for the period 1 January 2003 to 7 April 2012 using height-resolved limb spectra measured with the SCanning Imaging Absorption SpectroMeter for Atmospheric CHartographY (SCIAMACHY) on board ENVISAT (ENVIronmental SATellite). In this study, we present the retrieval code SCODA (SCIAMACHY cloud detection algorithm) based on a colour index method and test the accuracy of the retrieved CTHs in comparison to other methods. Sensitivity studies using the radiative transfer model SCIATRAN show that the method is capable of detecting cloud tops down to about 5 km and very thin cirrus clouds up to the tropopause. Volcanic particles can be detected that occasionally reach the lower stratosphere. Upper tropospheric ice clouds are observable for a nadir cloud optical thickness (COT)  ≥  0.01, which is in the subvisual range. This detection sensitivity decreases towards the lowermost troposphere. The COT detection limit for a water cloud top height of 5 km is roughly 0.1. This value is much lower than thresholds reported for passive cloud detection methods in nadir-viewing direction. Low clouds at 2 to 3 km can only be retrieved under very clean atmospheric conditions, as light scattering of aerosol particles interferes with the cloud particle scattering. We compare co-located SCIAMACHY limb and nadir cloud parameters that are retrieved with the Semi-Analytical CloUd Retrieval Algorithm (SACURA). Only opaque clouds (τN,c > 5) are detected with the nadir passive retrieval technique in the UV–visible and infrared wavelength ranges. Thus, due to the frequent occurrence of thin clouds and subvisual cirrus clouds in the tropics, larger CTH deviations are detected between both viewing geometries. Zonal mean CTH differences can be as high as 4 km in the tropics. The agreement in global cloud fields is sufficiently good. However, the land–sea contrast, as seen in nadir cloud occurrence frequency distributions, is not observed in limb geometry. Co-located cloud top height measurements of the limb-viewing Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on ENVISAT are compared for the period from January 2008 to March 2012. The global CTH agreement of about 1 km is observed, which is smaller than the vertical field of view of both instruments. Lower stratospheric aerosols from volcanic eruptions occasionally interfere with the cloud retrieval and inhibit the detection of tropospheric clouds. The aerosol impact on cloud retrievals was studied for the volcanoes Kasatochi (August 2008), Sarychev Peak (June 2009), and Nabro (June 2011). Long-lasting aerosol scattering is detected after these events in the Northern Hemisphere for heights above 12.5 km in tropical and polar latitudes. Aerosol top heights up to about 22 km are found in 2009 and the enhanced lower stratospheric aerosol layer persisted for about 7 months. In August 2009 about 82 % of the lower stratosphere between 30 and 70° N was filled with scattering particles and nearly 50 % in October 2008.


2017 ◽  
Vol 114 (27) ◽  
pp. 6972-6977 ◽  
Author(s):  
Pengfei Yu ◽  
Karen H. Rosenlof ◽  
Shang Liu ◽  
Hagen Telg ◽  
Troy D. Thornberry ◽  
...  

An enhanced aerosol layer near the tropopause over Asia during the June–September period of the Asian summer monsoon (ASM) was recently identified using satellite observations. Its sources and climate impact are presently not well-characterized. To improve understanding of this phenomenon, we made in situ aerosol measurements during summer 2015 from Kunming, China, then followed with a modeling study to assess the global significance. The in situ measurements revealed a robust enhancement in aerosol concentration that extended up to 2 km above the tropopause. A climate model simulation demonstrates that the abundant anthropogenic aerosol precursor emissions from Asia coupled with rapid vertical transport associated with monsoon convection leads to significant particle formation in the upper troposphere within the ASM anticyclone. These particles subsequently spread throughout the entire Northern Hemispheric (NH) lower stratosphere and contribute significantly (∼15%) to the NH stratospheric column aerosol surface area on an annual basis. This contribution is comparable to that from the sum of small volcanic eruptions in the period between 2000 and 2015. Although the ASM contribution is smaller than that from tropical upwelling (∼35%), we find that this region is about three times as efficient per unit area and time in populating the NH stratosphere with aerosol. With a substantial amount of organic and sulfur emissions in Asia, the ASM anticyclone serves as an efficient smokestack venting aerosols to the upper troposphere and lower stratosphere. As economic growth continues in Asia, the relative importance of Asian emissions to stratospheric aerosol is likely to increase.


2016 ◽  
Vol 16 (22) ◽  
pp. 14357-14369 ◽  
Author(s):  
Michael Höpfner ◽  
Rainer Volkamer ◽  
Udo Grabowski ◽  
Michel Grutter ◽  
Johannes Orphal ◽  
...  

Abstract. Ammonia (NH3) has been detected in the upper troposphere by the analysis of averaged MIPAS (Michelson Interferometer for Passive Atmospheric Sounding) infrared limb-emission spectra. We have found enhanced amounts of NH3 within the region of the Asian summer monsoon at 12–15 km altitude. Three-monthly, 10° longitude  ×  10° latitude average profiles reaching maximum mixing ratios of around 30 pptv in this altitude range have been retrieved, with a vertical resolution of 3–8 km and estimated errors of about 5 pptv. These observations show that loss processes during transport from the boundary layer to the upper troposphere within the Asian monsoon do not deplete the air entirely of NH3. Thus, ammonia might contribute to the so-called Asian tropopause aerosol layer by the formation of ammonium aerosol particles. On a global scale, outside the monsoon area and during different seasons, we could not detect enhanced values of NH3 above the actual detection limit of about 3–5 pptv. This upper bound helps to constrain global model simulations.


2020 ◽  
Vol 20 (7) ◽  
pp. 4105-4132 ◽  
Author(s):  
Timo Keber ◽  
Harald Bönisch ◽  
Carl Hartick ◽  
Marius Hauck ◽  
Fides Lefrancois ◽  
...  

Abstract. We present novel measurements of five short-lived brominated source gases (CH2Br2, CHBr3, CH2ClBr, CHCl2Br and CHClBr2). These rather short-lived gases are an important source of bromine to the stratosphere, where they can lead to depletion of ozone. The measurements have been obtained using an in situ gas chromatography and mass spectrometry (GC–MS) system on board the High Altitude and Long Range Research Aircraft (HALO). The instrument is extremely sensitive due to the use of chemical ionization, allowing detection limits in the lower parts per quadrillion (ppq, 10−15) range. Data from three campaigns using HALO are presented, where the upper troposphere and lower stratosphere (UTLS) of the northern hemispheric mid-to-high latitudes were sampled during winter and during late summer to early fall. We show that an observed decrease with altitude in the stratosphere is consistent with the relative lifetimes of the different compounds. Distributions of the five source gases and total organic bromine just below the tropopause show an increase in mixing ratio with latitude, in particular during polar winter. This increase in mixing ratio is explained by increasing lifetimes at higher latitudes during winter. As the mixing ratios at the extratropical tropopause are generally higher than those derived for the tropical tropopause, extratropical troposphere-to-stratosphere transport will result in elevated levels of organic bromine in comparison to air transported over the tropical tropopause. The observations are compared to model estimates using different emission scenarios. A scenario with emissions mainly confined to low latitudes cannot reproduce the observed latitudinal distributions and will tend to overestimate organic bromine input through the tropical tropopause from CH2Br2 and CHBr3. Consequently, the scenario also overestimates the amount of brominated organic gases in the stratosphere. The two scenarios with the highest overall emissions of CH2Br2 tend to overestimate mixing ratios at the tropical tropopause, but they are in much better agreement with extratropical tropopause mixing ratios. This shows that not only total emissions but also latitudinal distributions in the emissions are of importance. While an increase in tropopause mixing ratios with latitude is reproduced with all emission scenarios during winter, the simulated extratropical tropopause mixing ratios are on average lower than the observations during late summer to fall. We show that a good knowledge of the latitudinal distribution of tropopause mixing ratios and of the fractional contributions of tropical and extratropical air is needed to derive stratospheric inorganic bromine in the lowermost stratosphere from observations. In a sensitivity study we find maximum differences of a factor 2 in inorganic bromine in the lowermost stratosphere from source gas injection derived from observations and model outputs. The discrepancies depend on the emission scenarios and the assumed contributions from different source regions. Using better emission scenarios and reasonable assumptions on fractional contribution from the different source regions, the differences in inorganic bromine from source gas injection between model and observations is usually on the order of 1 ppt or less. We conclude that a good representation of the contributions of different source regions is required in models for a robust assessment of the role of short-lived halogen source gases on ozone depletion in the UTLS.


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