Active learning molecular beam epitaxy of complex quantum materials

Abstract

The integration of machine learning (ML) into materials science offers a transformative pathway toward fully autonomous synthesis workflows. For precise thin-film deposition techniques like molecular beam epitaxy (MBE), this automation is critical to overcome the time-consuming, manual navigation of high-dimensional thermodynamic phase spaces. Existing approaches for ML-assisted thin film growth predominantly rely on continuous Bayesian optimization (BO) models that assume smooth parameter landscapes. Consequently, they struggle to capture the abrupt crystallographic phase boundaries and narrow growth windows inherent to binary quantum materials. Here, we demonstrate an active learning protocol based on Sequential Model-Based Optimization (SMBO) designed specifically for the closed-loop MBE of such compounds. To overcome the limitations of continuous models while retaining the efficient exploration-exploitation logic of traditional BO, we combine a random forest surrogate model capable of capturing highly non-linear phase transitions and thermodynamics constraints of the growth process with an expected improvement function to predict optimum growth parameters. We apply this combined SMBO framework to the MBE of the topological Weyl ferromagnet Fe$_3$Sn, which exists as a metastable line compound. Using a small initial training set of fewer than twenty growth iterations, our active learning loop rapidly navigates a complex optimization landscape to identify an optimum growth window bounded by sharp transitions. Within only four active learning iterations, the absolute predictive error is halved to $\approx10\%$. This data-efficient framework paves the way for the autonomous discovery and thin-film synthesis of functional quantum materials.