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...

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Main Authors: Johan Friberg, Bengt G. Martinsson, Sandra M. Andersson, Carl A. M. Brenninkmeijer, Markus Hermann, Peter F. J. Van Velthoven, Andreas Zahn
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
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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.
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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
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