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The naturally existing chalcogenide Bi2Se3 is topologically nontrivial due tothe band inversion caused by strong spin-orbit coupling inside the bulk of thematerial. The surface states are spin polarized, protected by thetime-inversion symmetry, and thus robust to the scattering caused bynon-magnetic defects. A high purity topological insulator thin film can beeasily grown via molecular beam epitaxy (MBE) on various substrates to enablenovel electronics, optics, and spintronics applications. However, the uniquesurface state properties have historically been limited by the film quality,which is evaluated by crystallinity, surface morphology, and transport data.Here we propose and investigate different MBE growth strategies to improve thequality of Bi2Se3 thin films grown by MBE. In addition, growths of topologicaltrivial insulator (Bi0.5In0.5)2Se3 (BIS) are also investigated. BIS is oftenused as a buffer layer or separation layer for topological insulatorheterostructures. Based on the surface passivation status, we have classifiedthe substrates into two categories, self-passivated or unpassivated, anddetermine the optimal growth mechanisms on the representative sapphire andGaAs, respectively. Growth temperature is a crucial control parameter for thevan der Waals epitaxy for both types of substrates. For Bi2Se3 on GaAs, thesurface passivation status determines the dominant growth mechanism.

Optimization of the growth of the van der Waals materials Bi2Se3 and (Bi0.5In0.5)2Se3 by molecular beam epitaxy