Learning Atom Probe Tomography time-of-flight peaks for mass-to-charge ratio spectrometry

Ultramicroscopy. 2022 Jul:237:113521. doi: 10.1016/j.ultramic.2022.113521. Epub 2022 Apr 2.

Abstract

In laser-assisted atom probe tomography, an important goal is to reconstruct the mass-to-charge ratio, (m/z), spectrum due to various ion species. In general, the probability mass function (pmf) associated with the time-of-flight (TOF) spectrum produced by each ion species is unknown and varies from species-to-species. Moreover, measuring pmfs for distinct ion species in calibration experiments is not practical. Here, we present a mixture model method to determine TOF pmfs that can vary from peak-to-peak. In this approach, we determine weights of candidate pmfs with a maximum likelihood method. In a proof-of-principle study, we apply our method to a TOF spectrum acquired from a silicon sample and determine intensity estimates of singly charged isotopes of silicon.

Keywords: Atom Probe Tomography; Cross-validation; Expectation Maximization algorithm; Machine learning; Maximum likelihood; Mixture model; Silicon isotopes.