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https://doi.org/10.5194/amt-2017-288
© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 4.0 License.
Research article
06 Sep 2017
Review status
This discussion paper is a preprint. It is a manuscript under review for the journal Atmospheric Measurement Techniques (AMT).
Comparison of three aerosol chemical characterization techniques utilizing PTR-ToF-MS: A study on freshly formed and aged biogenic SOA
Georgios I. Gkatzelis1, Ralf Tillmann1, Thorsten Hohaus1, Markus Müller2,4, Philipp Eichler2, Kang-Ming Xu3, Patrick Schlag1, Sebastian H. Schmitt1, Robert Wegener1, Martin Kaminski1, Rupert Holzinger3, Armin Wisthaler2,5, and Astrid Kiendler-Scharr1 1Institute of Energy and Climate Research, IEK-8: Troposphere, Forschungszentrum Jülich GmbH, Jülich, Germany
2Institut für Ionenphysik und Angewandte Physik, Universität Innsbruck, Innsbruck, Austria
3Institute for Marine and Atmospheric research Utrecht, Princetonplein 5, 3584 CC, Utrecht, The Netherlands
4Ionicon Analytik GmbH, Innsbruck, Austria
5Department of Chemistry, University of Oslo, Norway
Abstract. An inter-comparison of different aerosol chemical characterization techniques has been performed as part of a chamber study of biogenic SOA formation and aging at the atmosphere simulation chamber SAPHIR. Three different aerosol sampling techniques, the aerosol collection module (ACM), the chemical analysis of aerosol on-line (CHARON) and the collection thermal desorption unit (TD) were connected to Proton Transfer Reaction Time of Flight Mass Spectrometers (PTR-ToF-MS) to provide chemical characterization of the SOA. The techniques were compared among each other and to results from an Aerosol Mass Spectrometer (AMS) and a Scanning Mobility Particle Sizer (SMPS). The experiments investigated SOA formation from the ozonolysis of β-pinene, limonene, a β-pinene/limonene mix and real plant emissions from Pinus sylvestris L. (Scots pine). The SOA was subsequently aged by photooxidation except for limonene SOA which was aged by NO3 oxidation.

Despite significant differences in the aerosol collection and desorption methods of the PTR based techniques, the determined chemical composition, i.e. the same major contributing signals were found by all instruments for the different chemical systems studied. These signals could be attributed to known products expected from the oxidation of the examined monoterpenes. The sampling and desorption method of ACM and TD, provided additional information on the volatility of individual compounds and showed relatively good agreement.

Averaged over all experiments, the total aerosol mass recovery compared to an SMPS varied from 80 ± 10 %, 51 ± 5 % and 27 ± 3 % for CHARON, ACM and TD, respectively. Comparison to the oxygen to carbon ratios (O : C) obtained by AMS showed that all PTR based techniques observed lower O : C ratios indicating a loss of molecular oxygen either during aerosol sampling or detection. The differences in total mass recovery and O : C between the three instruments resulted predominately from differences in the field strength (E/N) in the drift-tube reaction ionization chambers of the PTR-ToF-MS instruments and from dissimilarities in the collection/desorption of aerosols. Laboratory case studies showed that PTR-ToF-MS E/N conditions influenced fragmentation which resulted in water loss and carbon-oxygen bond breakage of the detected molecules. Since ACM and TD were operated in higher E/N compared to CHARON this resulted to higher fragmentation, thus affecting primarily the detected oxygen and carbon content and therefore also the mass recovery. Overall, these techniques have been shown to provide valuable insight on the chemical characteristics of BSOA, and can address unknown thermodynamic properties such as partitioning coefficient values and volatility patterns down to a compound specific level.


Citation: Gkatzelis, G. I., Tillmann, R., Hohaus, T., Müller, M., Eichler, P., Xu, K.-M., Schlag, P., Schmitt, S. H., Wegener, R., Kaminski, M., Holzinger, R., Wisthaler, A., and Kiendler-Scharr, A.: Comparison of three aerosol chemical characterization techniques utilizing PTR-ToF-MS: A study on freshly formed and aged biogenic SOA, Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2017-288, in review, 2017.
Georgios I. Gkatzelis et al.
Georgios I. Gkatzelis et al.
Georgios I. Gkatzelis et al.

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Short summary
This manuscript presents an inter-comparison of state of the art online and in situ particle sampling techniques connected to proton transfer reaction time of flight mass spectrometry (PTR-ToF-MS). Collection and vaporization of aerosol combined with soft ionization mass spectrometry offers the advantage of detailed chemical characterization of SOA species. The benefits of these techniques are highlighted through their consistency in providing the chemical composition of biogenic SOA.
This manuscript presents an inter-comparison of state of the art online and in situ particle...
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