Sources of increase in lowermost stratospheric sulphurous and carbonaceous aerosol background concentrations during 1999–2008 derived from CARIBIC flights
This study focuses on sulphurous and carbonaceous aerosol, the major constituents of particulate matter in the lowermost stratosphere (LMS), based on in situ measurements from 1999 to 2008. Aerosol particles in the size range of 0.08–2 µm were collected monthly during intercontinental flights with t...
Main Authors: | , , , , , , |
---|---|
Format: | Article |
Language: | English |
Published: |
Stockholm University Press
2014-03-01
|
Series: | Tellus: Series B, Chemical and Physical Meteorology |
Subjects: | |
Online Access: | http://www.tellusb.net/index.php/tellusb/article/download/23428/pdf_1 |
_version_ | 1828528114870779904 |
---|---|
author | Johan Friberg Bengt G. Martinsson Sandra M. Andersson Carl A. M. Brenninkmeijer Markus Hermann Peter F. J. Van Velthoven Andreas Zahn |
author_facet | Johan Friberg Bengt G. Martinsson Sandra M. Andersson Carl A. M. Brenninkmeijer Markus Hermann Peter F. J. Van Velthoven Andreas Zahn |
author_sort | Johan Friberg |
collection | DOAJ |
description | This study focuses on sulphurous and carbonaceous aerosol, the major constituents of particulate matter in the lowermost stratosphere (LMS), based on in situ measurements from 1999 to 2008. Aerosol particles in the size range of 0.08–2 µm were collected monthly during intercontinental flights with the CARIBIC passenger aircraft, presenting the first long-term study on carbonaceous aerosol in the LMS. Elemental concentrations were derived via subsequent laboratory-based ion beam analysis. The stoichiometry indicates that the sulphurous fraction is sulphate, while an O/C ratio of 0.2 indicates that the carbonaceous aerosol is organic. The concentration of the carbonaceous component corresponded on average to approximately 25% of that of the sulphurous, and could not be explained by forest fires or biomass burning, since the average mass ratio of Fe to K was 16 times higher than typical ratios in effluents from biomass burning. The data reveal increasing concentrations of particulate sulphur and carbon with a doubling of particulate sulphur from 1999 to 2008 in the northern hemisphere LMS. Periods of elevated concentrations of particulate sulphur in the LMS are linked to downward transport of aerosol from higher altitudes, using ozone as a tracer for stratospheric air. Tropical volcanic eruptions penetrating the tropical tropopause are identified as the likely cause of the particulate sulphur and carbon increase in the LMS, where entrainment of lower tropospheric air into volcanic jets and plumes could be the cause of the carbon increase. |
first_indexed | 2024-12-11T21:47:50Z |
format | Article |
id | doaj.art-4cc1ee20cb264662974bef0d240c8f48 |
institution | Directory Open Access Journal |
issn | 1600-0889 |
language | English |
last_indexed | 2024-12-11T21:47:50Z |
publishDate | 2014-03-01 |
publisher | Stockholm University Press |
record_format | Article |
series | Tellus: Series B, Chemical and Physical Meteorology |
spelling | doaj.art-4cc1ee20cb264662974bef0d240c8f482022-12-22T00:49:33ZengStockholm University PressTellus: Series B, Chemical and Physical Meteorology1600-08892014-03-0166011510.3402/tellusb.v66.2342823428Sources of increase in lowermost stratospheric sulphurous and carbonaceous aerosol background concentrations during 1999–2008 derived from CARIBIC flightsJohan Friberg0Bengt G. Martinsson1Sandra M. Andersson2Carl A. M. Brenninkmeijer3Markus Hermann4Peter F. J. Van Velthoven5Andreas Zahn6 Department of Physics, Lund University, Lund, Sweden Department of Physics, Lund University, Lund, Sweden Department of Physics, Lund University, Lund, Sweden Max Planck Institute for Chemistry, Mainz, Germany Leibniz Institute for Tropospheric Research, Leipzig, Germany Royal Netherlands Meteorological Institute, de Bilt, The Netherlands Institute for Meteorology and Climate Research, Karlsruhe Institute of Technology (KIT), Karlsruhe, GermanyThis study focuses on sulphurous and carbonaceous aerosol, the major constituents of particulate matter in the lowermost stratosphere (LMS), based on in situ measurements from 1999 to 2008. Aerosol particles in the size range of 0.08–2 µm were collected monthly during intercontinental flights with the CARIBIC passenger aircraft, presenting the first long-term study on carbonaceous aerosol in the LMS. Elemental concentrations were derived via subsequent laboratory-based ion beam analysis. The stoichiometry indicates that the sulphurous fraction is sulphate, while an O/C ratio of 0.2 indicates that the carbonaceous aerosol is organic. The concentration of the carbonaceous component corresponded on average to approximately 25% of that of the sulphurous, and could not be explained by forest fires or biomass burning, since the average mass ratio of Fe to K was 16 times higher than typical ratios in effluents from biomass burning. The data reveal increasing concentrations of particulate sulphur and carbon with a doubling of particulate sulphur from 1999 to 2008 in the northern hemisphere LMS. Periods of elevated concentrations of particulate sulphur in the LMS are linked to downward transport of aerosol from higher altitudes, using ozone as a tracer for stratospheric air. Tropical volcanic eruptions penetrating the tropical tropopause are identified as the likely cause of the particulate sulphur and carbon increase in the LMS, where entrainment of lower tropospheric air into volcanic jets and plumes could be the cause of the carbon increase.http://www.tellusb.net/index.php/tellusb/article/download/23428/pdf_1lowermost stratosphereelemental compositionvolcanic aerosolsulphurous aerosolcarbonaceous aerosol |
spellingShingle | Johan Friberg Bengt G. Martinsson Sandra M. Andersson Carl A. M. Brenninkmeijer Markus Hermann Peter F. J. Van Velthoven Andreas Zahn Sources of increase in lowermost stratospheric sulphurous and carbonaceous aerosol background concentrations during 1999–2008 derived from CARIBIC flights Tellus: Series B, Chemical and Physical Meteorology lowermost stratosphere elemental composition volcanic aerosol sulphurous aerosol carbonaceous aerosol |
title | Sources of increase in lowermost stratospheric sulphurous and carbonaceous aerosol background concentrations during 1999–2008 derived from CARIBIC flights |
title_full | Sources of increase in lowermost stratospheric sulphurous and carbonaceous aerosol background concentrations during 1999–2008 derived from CARIBIC flights |
title_fullStr | Sources of increase in lowermost stratospheric sulphurous and carbonaceous aerosol background concentrations during 1999–2008 derived from CARIBIC flights |
title_full_unstemmed | Sources of increase in lowermost stratospheric sulphurous and carbonaceous aerosol background concentrations during 1999–2008 derived from CARIBIC flights |
title_short | Sources of increase in lowermost stratospheric sulphurous and carbonaceous aerosol background concentrations during 1999–2008 derived from CARIBIC flights |
title_sort | sources of increase in lowermost stratospheric sulphurous and carbonaceous aerosol background concentrations during 1999 2008 derived from caribic flights |
topic | lowermost stratosphere elemental composition volcanic aerosol sulphurous aerosol carbonaceous aerosol |
url | http://www.tellusb.net/index.php/tellusb/article/download/23428/pdf_1 |
work_keys_str_mv | AT johanfriberg sourcesofincreaseinlowermoststratosphericsulphurousandcarbonaceousaerosolbackgroundconcentrationsduring19992008derivedfromcaribicflights AT bengtgmartinsson sourcesofincreaseinlowermoststratosphericsulphurousandcarbonaceousaerosolbackgroundconcentrationsduring19992008derivedfromcaribicflights AT sandramandersson sourcesofincreaseinlowermoststratosphericsulphurousandcarbonaceousaerosolbackgroundconcentrationsduring19992008derivedfromcaribicflights AT carlambrenninkmeijer sourcesofincreaseinlowermoststratosphericsulphurousandcarbonaceousaerosolbackgroundconcentrationsduring19992008derivedfromcaribicflights AT markushermann sourcesofincreaseinlowermoststratosphericsulphurousandcarbonaceousaerosolbackgroundconcentrationsduring19992008derivedfromcaribicflights AT peterfjvanvelthoven sourcesofincreaseinlowermoststratosphericsulphurousandcarbonaceousaerosolbackgroundconcentrationsduring19992008derivedfromcaribicflights AT andreaszahn sourcesofincreaseinlowermoststratosphericsulphurousandcarbonaceousaerosolbackgroundconcentrationsduring19992008derivedfromcaribicflights |