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This dissertation, "Molecular Beam Epitaxy of Three Dimensional Topological Insulator Bi₂Se₃ Thin Films" by Xin, Guo,, was obtained from The University of Hong Kong (Pokfulam, Hong Kong) and is being sold pursuant to Creative Commons: Attribution 3.0 Hong Kong License. The content of this dissertation has not been altered in any way. We have altered the formatting in order to facilitate the ease of printing and reading of the dissertation. All rights not granted by the above license are retained by the author. Abstract: In this thesis, molecular-beam epitaxy (MBE) of three-dimensional (3D) topological insulator (TI) Bi_2 Se_3 thin films on different substrates is presented. The substrates experimented include InP(111)A, GaAs(111)A, InP(001) and GaAs(001). Multiple characterization techniques are employed to investigate the film's structural, morphological and electrical properties. To facilitate growth of high quality epitaxial Bi_2 Se_3, thermal treatment of the substrate surfaceturnsout to be crucial for both InP(001) and InP(111). On the other hand, for high-index epitaxial Bi_2 Se_3 growth on GaAs(001), the In_2 Se_3 buffer layer has to be employed. Twin defects in epitaxial Bi_2 Se_3 (111) thin films on hexagonal substrates have been found inevitable in the past. In this study, however, such defects are successfully suppressed on InP(111)A and GaAs(111)Asubstrates, as evidenced in electron diffraction and morphological measurements. The prerequisite for the twin-free Bi_2 Se_3 (111) epitaxy appears to be the step-flow growth mode on the purposely treated stepped substrate surfaces, where deposits incorporate in film at step edges. The lattice of InP or GaAs substrate then plays a guiding role for epitaxial Bi_2 Se_3. Twin suppression is also seen to occur for growth on vicinal and islanded InP(111)A substrate, where a high density of steps inherently exists on surface. Transport studies on such single-domain Bi2Se3epifilms show superior electronic