Machine learning enhanced atom probe tomography analysis: a snapshot review

Atom probe tomography (APT) is a burgeoning characterization technique that provides compositional mapping of materials in three-dimensions at near-atomic scale. Since its significant expansion in the past 30 years, we estimate that one million APT datasets have been collected, each containing millions to billions of individual ions. Their analysis and the extraction of microstructural information has largely relied upon individual users whose varied level of expertise causes clear and documented bias. Current practices hinder efficient data processing, and make challenging standardization and the deployment of data analysis workflows that would be compliant with FAIR data principles. Over the past decade, building upon the long-standing expertise of the APT community in the development of advanced data processing or data mining techniques, there has been a surge of novel machine learning (ML) approaches aiming for user-independence, and that are efficient, reproducible, and robust from a statistics perspective. Here, we provide a snapshot review of this rapidly evolving field. We begin with a brief introduction to APT and the nature of the APT data. This is followed by an overview of relevant ML algorithms and a comprehensive review of their applications to APT. We also discuss how ML can enable discoveries beyond human capability, offering new insights into the mechanisms within materials. Finally, we provide guidance for future directions in this domain.

Machine-learning-enhanced time-of-flight mass spectrometry analysis

Mass spectrometry is a widespread approach to work out what are the constituents of a material. Atoms and molecules are removed from the material and collected, and subsequently, a critical step is to infer their correct identities based from patterns formed in their mass-to-charge ratios and relative isotopic abundances. However, this identification step still mainly relies on individual user's expertise, making its standardization challenging, and hindering efficient data processing. Here, we introduce an approach that leverages modern machine learning technique to identify peak patterns in time-of-flight mass spectra within microseconds, outperforming human users without loss of accuracy. Our approach is cross-validated on mass spectra generated from different time-of-flight mass spectrometry(ToF-MS) techniques, offering the ToF-MS community an open-source, intelligent mass spectra analysis.

On Open and Strong-Scaling Tools for Atom Probe Crystallography: High-Throughput Methods for Indexing Crystal Structure and Orientation

Volumetric crystal structure indexing and orientation mapping are key data processing steps for virtually any quantitative study of spatial correlations between the local chemistry and the microstructure of a material. For electron and X-ray diffraction methods it is possible to develop indexing tools which compare measured and analytically computed patterns to decode the structure and relative orientation within local regions of interest. Consequently, a number of numerically efficient and automated software tools exist to solve the above characterisation tasks. For atom probe tomography (APT) experiments, however, the strategy of making comparisons between measured and analytically computed patterns is less robust because many APT datasets may contain substantial noise. Given that general enough predictive models for such noise remain elusive, crystallography tools for APT face several limitations: Their robustness to noise, and therefore, their capability to identify and distinguish different crystal structures and orientation is limited. In addition, the tools are sequential and demand substantial manual interaction. In combination, this makes robust uncertainty quantifying with automated high-throughput studies of the latent crystallographic information a difficult task with APT data. To improve the situation, we review the existent methods and discuss how they link to those in the diffraction communities. With this we modify some of the APT methods to yield more robust descriptors of the atomic arrangement. We report how this enables the development of an open-source software tool for strong-scaling and automated identifying of crystal structure and mapping crystal orientation in nanocrystalline APT datasets with multiple phases.