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© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.

Submitted as: research article 20 Jan 2020

Submitted as: research article | 20 Jan 2020

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This preprint is currently under review for the journal ACP.

Resonance-Enhanced Detection of Metals in Aerosols using Single Particle Mass Spectrometry

Johannes Passig1,2,3, Julian Schade2,3, Ellen Iva Rosewig2,3, Robert Irsig3,4, Thomas Kröger-Badge2,3, Hendryk Czech1,2,3, Martin Sklorz1, Thorsten Streibel1,2, Lei Li5, Xue Li5, Zhen Zhou5, Henrik Fallgren6, Jana Moldanova6, and Ralf Zimmermann1,2,3 Johannes Passig et al.
  • 1Joint Mass Spectrometry Centre, Cooperation Group Comprehensive Molecular Analytics (CMA), Helmholtz Zentrum München, 85764 Neuherberg, Germany
  • 2Joint Mass Spectrometry Centre, Chair of Analytical Chemistry, University Rostock, 18059 Rostock, Germany
  • 3Department Life, Light & Matter, University of Rostock, 18051 Rostock, Germany
  • 4Photonion GmbH, 19061 Schwerin, Germany
  • 5Institute of Mass Spectrometry and Atmospheric Environment, Jinan University, Guangzhou 510632, China and Guangzhou Hexin Instrument Co., LTD, Guangzhou 510530, China
  • 6IVL Swedish Environmental Research Institute, 411 33 Gothenburg, Sweden

Abstract. We describe resonance effects in laser desorption/ionization (LDI) of particles that substantially increase the sensitivity and selectivity to metals in single particle mass spectrometry (SPMS). Within the proposed scenario, resonant light absorption by ablated metal atoms increases their ionization rate within a single laser pulse. By choosing the appropriate laser wavelength, the key micronutrients Fe, Zn and Mn can be detected on individual aerosol particles with considerably improved efficiency. These ionization enhancements for metals apply to natural dust and anthropogenic aerosols, both important sources of bioavailable metals to marine environments. Transferring the results into applications, we show that the spectrum of our KrF-excimer laser is in resonance with a major absorption line of iron atoms. To estimate the impact of resonant LDI on the metal detection efficiency in SPMS applications, we performed a field experiment on ambient air with two alternately firing excimer lasers of different wavelengths. Herein, resonant LDI with the KrF-excimer laser (248.3 nm) revealed Fe signatures for many more aerosol particles compared to the more common ArF-excimer laser line of 193.3 nm. Moreover, resonant ionization of iron appeared to be less dependent on the particle matrix than conventional non-resonant LDI, allowing a more universal and secure detection of Fe. Our findings show a way to improve the detection and source attribution capabilities of SPMS for particle-bound metals, a health-relevant aerosol component and an important source of micronutrients to the surface oceans affecting marine primary productivity.

Johannes Passig et al.

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Johannes Passig et al.

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Publications Copernicus
Short summary
Particle-bound metals in both natural dusts and polluted air can induce severe health effects. They are also transported by the wind into the oceans, provide micronutrients and thus modulate biodiversity, fishery and climate. We show a way to more efficiently detect metals in individual particles, while preserving source information. Our detection scheme is less dependent on the particle type and its atmospheric changes, and thus a valuable tool to study biogechemical cycles and air pollution.
Particle-bound metals in both natural dusts and polluted air can induce severe health effects....