Laser-driven ionization mechanisms of aluminum for single particle aerosol mass spectrometry

Lietz, Amanda M.; Yee, Benjamin T.; Musk II, Jeffrey; Moffat, Harry K.; Wiemann, Dora K.; Settecerri, Taylor; Fergenson, David; Omana, Michael A.; Hopkins, Matthew M.

doi:10.1016/j.sab.2022.106543

Laser-driven ionization mechanisms of aluminum for single particle aerosol mass spectrometry

Journal Article · Fri Oct 14 00:00:00 EDT 2022 · Spectrochimica Acta. Part B, Atomic Spectroscopy

DOI:https://doi.org/10.1016/j.sab.2022.106543· OSTI ID:1894615

Lietz, Amanda M. ^[1]; Yee, Benjamin T. ^[1]; Musk II, Jeffrey ^[1]; Moffat, Harry K. ^[1]; Wiemann, Dora K. ^[1]; Settecerri, Taylor ^[1]; Fergenson, David ^[2]; Omana, Michael A. ^[1]; Hopkins, Matthew M. ^[1]

Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)
Livermore Instruments, Oakland, CA (United States)

Single particle aerosol mass spectrometry (SPAMS), an analytical technique for measuring the size and composition of individual micron-scale particles, is capable of analyzing atmospheric pollutants and bioaerosols much more efficiently and with more detail than conventional methods which require the collection of particles onto filters for analysis in the laboratory. Despite SPAMS’ demonstrated capabilities, the primary mechanisms of ionization are not fully understood, which creates challenges in optimizing and interpreting SPAMS signals. In this paper, we present a well-stirred reactor model for the reactions involved with the laser-induced vaporization and ionization of an individual particle. The SPAMS conditions modeled in this paper include a 248 nm laser which is pulsed for 8 ns to vaporize and ionize each particle in vacuum. The ionization of 1 μm, spherical Al particles was studied by approximating them with a 0-dimensional plasma chemistry model. The primary mechanism of absorption of the 248 nm photons was pressure-broadened direct photoexcitation to Al(y²D). Atoms in this highly excited state then undergo superelastic collisions with electrons, heating the electrons and populating the lower energy excited states. We found that the primary ionization mechanism is electron impact ionization of various excited state Al atoms, especially Al(y²D). Because the gas expands rapidly into vacuum, its temperature decreases rapidly. The rate of three-body recombination (e^- + e^- + Al⁺ → Al + e^-) increases at low temperature, and most of the electrons and ions produced recombine within several μs of the laser pulse. The importance of the direct photoexcitation indicates that the relative peak heights of different elements in SPAMS mass spectra may be sensitive to the available photoexcitation transitions. We also discuss the effects of laser intensity, particle diameter, and expansion dynamics.

View Accepted Manuscript (DOE)

Research Organization:: Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)

Sponsoring Organization:: USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: NA0003525

OSTI ID:: 1894615

Alternate ID(s):: OSTI ID: 1961674

Report Number(s):: SAND2022-14059J; 710835

Journal Information:: Spectrochimica Acta. Part B, Atomic Spectroscopy, Journal Name: Spectrochimica Acta. Part B, Atomic Spectroscopy Vol. 197; ISSN 0584-8547

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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