Chemical composition and source attribution of sub-micrometre aerosol particles in the summertime Arctic lower troposphere

Publikationstyp:
Zeitschriftenaufsatz
Metadaten:
Autoren
  • Franziska Kollner
  • Johannes Schneider
  • Megan D Willis
  • Hannes Schulz
  • Daniel Kunkel
  • Heiko Bozem
  • Peter Hoor
  • Thomas Klimach
  • Frank Helleis
  • Julia Burkart
  • W Richard Leaitch
  • Amir A Aliabadi
  • Jonathan PD Abbatt
  • Andreas B Herber
  • Stephan Borrmann
Autoren-URL
https://www.webofscience.com/api/gateway?GWVersion=2&SrcApp=fis-test-1&SrcAuth=WosAPI&KeyUT=WOS:000646694000003&DestLinkType=FullRecord&DestApp=WOS_CPL
DOI
10.5194/acp-21-6509-2021
eISSN
1680-7324
Externe Identifier
  • Clarivate Analytics Document Solution ID: RW7IC
ISSN
1680-7316
Ausgabe der Veröffentlichung
8
Zeitschrift
ATMOSPHERIC CHEMISTRY AND PHYSICS
Paginierung
6509 - 6539
Datum der Veröffentlichung
2021
Status
Published
Titel
Chemical composition and source attribution of sub-micrometre aerosol particles in the summertime Arctic lower troposphere
Sub types
  • Article
Ausgabe der Zeitschrift
21

Datenquelle: Web of Science (Lite)

Andere Metadatenquellen:
Abstract
<jats:p>Abstract. Aerosol particles impact the Arctic climate system both directly and indirectly by modifying cloud properties, yet our understanding of their vertical distribution, chemical composition, mixing state, and sources in the summertime Arctic is incomplete. In situ vertical observations of particle properties in the high Arctic combined with modelling analysis on source attribution are in short supply, particularly during summer. We thus use airborne measurements of aerosol particle composition to demonstrate the strong contrast between particle sources and composition within and above the summertime Arctic boundary layer. In situ measurements from two complementary aerosol mass spectrometers, the Aircraft-based Laser Ablation Aerosol Mass Spectrometer (ALABAMA) and an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), are presented alongside black carbon measurements from an single particle soot photometer (SP2). Particle composition analysis was complemented by trace gas measurements, satellite data, and air mass history modelling to attribute particle properties to particle origin and air mass source regions. Particle composition above the summertime Arctic boundary layer was dominated by chemically aged particles, containing elemental carbon, nitrate, ammonium, sulfate, and organic matter. From our analysis, we conclude that the presence of these particles was driven by transport of aerosol and precursor gases from mid-latitudes to Arctic regions. Specifically, elevated concentrations of nitrate, ammonium, and organic matter coincided with time spent over vegetation fires in northern Canada. In parallel, those particles were largely present in high CO environments (&gt; 90 ppbv). Additionally, we observed that the organic-to-sulfate ratio was enhanced with increasing influence from these fires. Besides vegetation fires, particle sources in mid-latitudes further include anthropogenic emissions in Europe, North America, and East Asia. The presence of particles in the Arctic lower free troposphere, particularly sulfate, correlated with time spent over populated and industrial areas in these regions. Further, the size distribution of free tropospheric particles containing elemental carbon and nitrate was shifted to larger diameters compared to particles present within the boundary layer. Moreover, our analysis suggests that organic matter, when present in the Arctic free troposphere, can partly be identified as low molecular weight dicarboxylic acids (oxalic, malonic, and succinic acid). Particles containing dicarboxylic acids were largely present when the residence time of air masses outside Arctic regions was high. In contrast, particle composition within the marine boundary layer was largely driven by Arctic regional processes. Air mass history modelling demonstrated that alongside primary sea spray particles, marine biogenic sources contributed to secondary aerosol formation via trimethylamine, methanesulfonic acid, sulfate, and other organic species. Our findings improve our knowledge of mid-latitude and Arctic regional sources that influence the vertical distribution of particle chemical composition and mixing state in the Arctic summer. </jats:p>
Autoren
  • Franziska Köllner
  • Johannes Schneider
  • Megan D Willis
  • Hannes Schulz
  • Daniel Kunkel
  • Heiko Bozem
  • Peter Hoor
  • Thomas Klimach
  • Frank Helleis
  • Julia Burkart
  • W Richard Leaitch
  • Amir A Aliabadi
  • Jonathan PD Abbatt
  • Andreas B Herber
  • Stephan Borrmann
DOI
10.5194/acp-21-6509-2021
eISSN
1680-7324
Ausgabe der Veröffentlichung
8
Zeitschrift
Atmospheric Chemistry and Physics
Sprache
en
Online publication date
2021
Paginierung
6509 - 6539
Status
Published online
Herausgeber
Copernicus GmbH
Herausgeber URL
http://dx.doi.org/10.5194/acp-21-6509-2021
Datum der Datenerfassung
2021
Titel
Chemical composition and source attribution of sub-micrometre aerosol particles in the summertime Arctic lower troposphere
Ausgabe der Zeitschrift
21

Datenquelle: Crossref

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