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Intrinsic magnetic topological insulators have emerged as a promisingplatform to study the interplay between topological surface states andferromagnetism. This unique interplay can give rise to a variety of exoticquantum phenomena, including the quantum anomalous Hall effect and axioninsulating states. Here, utilizing molecular beam epitaxy (MBE), we present acomprehensive study of the growth of high-quality MnBi2Te4 thin films on Si(111), epitaxial graphene, and highly ordered pyrolytic graphite substrates. Bycombining a suite of in-situ characterization techniques, we obtain criticalinsights into the atomic-level control of MnBi2Te4 epitaxial growth. First, weextract the free energy landscape for the epitaxial relationship as a functionof the in-plane angular distribution. Then, by employing an optimizedlayer-by-layer growth, we determine the chemical potential and Dirac point ofthe thin film at different thicknesses. Overall, these results establish afoundation for understanding the growth dynamics of MnBi2Te4 and pave the wayfor the future applications of MBE in emerging topological quantum materials.

Atomistic Control in Molecular Beam Epitaxy Growth of Intrinsic Magnetic Topological Insulator MnBi2Te4