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Atmospheric Measurement Techniques An interactive open-access journal of the European Geosciences Union
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Discussion papers
https://doi.org/10.5194/amt-2019-45
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/amt-2019-45
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.

Research article 05 Mar 2019

Research article | 05 Mar 2019

Review status
This discussion paper is a preprint. It is a manuscript under review for the journal Atmospheric Measurement Techniques (AMT).

An Extractive Electrospray Ionization Time-of-Flight Mass Spectrometer (EESI-TOF) for online measurement of atmospheric aerosol particles

Felipe D. Lopez-Hilfiker1,a, Veronika Pospisilova1, Wei Huang2, Markus Kalberer3,4, Claudia Mohr5, Giulia Stefenelli1, Joel A. Thornton6, Urs Baltensperger1, Andre S. H. Prevot1, and Jay G. Slowik1 Felipe D. Lopez-Hilfiker et al.
  • 1Laboratory of Atmospheric Chemistry, Paul Scherrer Institute (PSI), 5232 VilligenPSI, Switzerland
  • 2Institute of Meteorology and Climate Research, Karlsruhe Institute of Technology, 76131 Karlsruhe, Germany
  • 3Department of Chemistry, University of Cambridge, Cambridge CB2 1EW, UK
  • 4Department of Environmental Sciences, University of Basel, 4056 Basel, Switzerland
  • 5Department of Environmental Science and Analytical Chemistry, Stockholm University, 106 91 Stockholm, Sweden
  • 6Department of Atmospheric Sciences, University of Washington, Seattle, WA 98195, Washington, USA
  • anow at:TofwerkAG, 3600 Thun, Switzerland

Abstract. Real-time, online measurements of atmospheric organic aerosol (OA) composition are an essential tool for determining the emissions sources and physicochemical processes governing aerosol effects on climate and health. However, the reliance of current techniques on thermal desorption, hard ionization, and/or separated collection/analysis stages introduces significant uncertainties into OA composition measurements, hindering progress towards these goals. To address this gap, we present a novel, field-deployable extractive electrospray ionization time-of-flight mass spectrometer (EESI-TOF), which provides online, near-molecular OA measurements at atmospherically relevant concentrations without analyte fragmentation or decomposition. Aerosol particles are continuously sampled into the EESI-TOF, where they intersect a spray of charged droplets generated by a conventional electrospray probe. Soluble components are extracted, and then ionized as the droplets are evaporated. The EESI-TOF achieves a linear response to mass, with detection limits on the order of 1 to 10 ng m−3 for typical atmospherically-relevant compounds. In contrast to conventional electrospray systems, the EESI-TOF response is not significantly affected by a changing OA matrix, while a slight decrease in sensitivity in response to increasing absolute humidity is observed for some ions. Although the relative sensitivities to a variety of commercially available organic standards vary by approximately a factor of 30, the bulk sensitivity to most SOA compounds varies by only a factor of 6. Further, the ratio of compound-by-compound sensitivities between the EESI-TOF and an iodide adduct FIGAERO-CIMS vary by only ± 50 %, suggesting that EESI-TOF mass spectra indeed reflect the actual distribution of detectable compounds in the particle phase. Successful deployments of the EESI-TOF for laboratory environmental chamber measurements, ground-based ambient sampling, and proof-of-concept measurements aboard a research aircraft highlight the versatility and potential of the EESI-TOF system.

Felipe D. Lopez-Hilfiker et al.
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Status: final response (author comments only)
Status: final response (author comments only)
AC: Author comment | RC: Referee comment | SC: Short comment | EC: Editor comment
Felipe D. Lopez-Hilfiker et al.
Felipe D. Lopez-Hilfiker et al.
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Short summary
We present a novel, field-deployable extractive electrospray time-of-flight mass spectrometer (EESI-TOF), which provides real-time, near-molecular measurements of organic aerosol at atmospherically relevant concentrations, addressing a critical gap in existing measurement capabilities. Successful deployments of the EESI-TOF for laboratory measurements, ground-based ambient sampling, and aboard a research aircraft highlight the versatility and potential of the EESI-TOF system.
We present a novel, field-deployable extractive electrospray time-of-flight mass spectrometer...
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