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Volume 15, issue 19
Atmos. Chem. Phys., 15, 11373–11398, 2015
© Author(s) 2015. This work is distributed under
the Creative Commons Attribution 3.0 License.
Atmos. Chem. Phys., 15, 11373–11398, 2015
© Author(s) 2015. This work is distributed under
the Creative Commons Attribution 3.0 License.

Research article 14 Oct 2015

Research article | 14 Oct 2015

Fourteen months of on-line measurements of the non-refractory submicron aerosol at the Jungfraujoch (3580 m a.s.l.) – chemical composition, origins and organic aerosol sources

R. Fröhlich1, M. J. Cubison2, J. G. Slowik1, N. Bukowiecki1, F. Canonaco1, P. L. Croteau3, M. Gysel1, S. Henne4, E. Herrmann1, J. T. Jayne3, M. Steinbacher4, D. R. Worsnop3, U. Baltensperger1, and A. S. H. Prévôt1 R. Fröhlich et al.
  • 1Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, Villigen PSI, Switzerland
  • 2Tofwerk AG, Thun, Switzerland
  • 3Aerodyne Research Inc., Billerica, Massachusetts, USA
  • 4Laboratory for Air Pollution/Environmental Technology, Empa, Swiss Federal Laboratories for Materials Science and Technology, Dübendorf, Switzerland

Abstract. Chemically resolved (organic, nitrate, sulfate, ammonium) data of non-refractory submicron (NR-PM1) aerosol from the first long-term deployment (27 July 2012 to 02 October 2013) of a time-of-flight aerosol chemical speciation monitor (ToF-ACSM) at the Swiss high-altitude site Jungfraujoch (JFJ; 3580 m a.s.l.) are presented. Besides total mass loadings, diurnal variations and relative species contributions during the different meteorological seasons, geographical origin and sources of organic aerosol (OA) are discussed. Backward transport simulations show that the highest (especially sulfate) concentrations of NR-PM1 were measured in air masses advected to the station from regions south of the JFJ, while lowest concentrations were seen from western regions. OA source apportionment for each season was performed using the Source Finder (SoFi) interface for the multilinear engine (ME-2). OA was dominated in all seasons by oxygenated OA (OOA, 71–88 %), with lesser contributions from local tourism-related activities (7–12 %) and hydrocarbon-like OA related to regional vertical transport (3–9 %). In summer the OOA can be separated into a background low-volatility OA (LV-OOA I, possibly associated with long-range transport) and a slightly less oxidised low-volatility OA (LV-OOA II) associated with regional vertical transport. Wood burning-related OA associated with regional transport was detected during the whole winter 2012/2013 and during rare events in summer 2013, in the latter case attributed to small-scale transport for the surrounding valleys. Additionally, the data were divided into periods with free tropospheric (FT) conditions and periods with planetary boundary layer (PBL) influence, enabling the assessment of the composition for each. Most nitrate and part of the OA are injected from the regional PBL, while sulfate is mainly produced in the FT. The south/north gradient of sulfate is also pronounced in FT air masses (sulfate mass fraction from the south: 45 %; from the north: 29 %). Furthermore, a detailed investigation of specific marker fragments of the OA spectra (f43, f44, f55, f57, f60) showed different degrees of ageing depending on season.

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Short summary
This manuscript presents the first long-term (14-month) and highly time-resolved (10 min) measurements of NR-PM1 aerosol chemical composition at a high-altitude site (JFJ, Switzerland, 3580m a.s.l.). The elevated location allowed the investigation of free tropospheric aerosol year round. Total and relative mass loadings, diurnal variations as well as seasonal variations are discussed together with geographical origin, organic aerosol sources and the influence of the planetary boundary layer.
This manuscript presents the first long-term (14-month) and highly time-resolved (10 min)...
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