Electronic and chemical phase identification in photoemission experiments using unsupervised machine learning

Abstract

Vacuum ultraviolet photoemission spectroscopies are very information-rich experiments, but due to their surface sensitivity, data are often collected on an initially uncharacterized surface. Traditional raster-grid approaches for locating optimal measurement regions can be time-consuming. In this work, we introduce AARDVARK, a generalizable framework for sample exploration that leverages dimensionality reduction and Gaussian process regression to guide initial sample searches in spatially-resolved photoemission experiments. By utilizing UMAP as a target for a Gaussian process, the algorithm efficiently identifies boundaries of spectroscopically distinct regions, dynamically adapting to variations in sample characteristics. The algorithm enables real-time decision making in measurement selection, optimizes data acquisition, and presents a robust framework for future autonomous sample exploration in photoemission experiments.