Topological Phase Control of Surface States in Bi2Se3 via Spin–Orbit Coupling Modulation through Interface Engineering between HfO2–X

The direct control of topological surface states in topological insulators is an important prerequisite for the application of these materials. Conventional attempts to utilize magnetic doping, mechanical tuning, structural engineering, external bias, and external magnetic fields suffer from a lack of reversible switching and have limited tunability. We demonstrate the direct control of topological phases in a bismuth selenide (Bi2Se3) topological insulator in 3 nm molecular beam epitaxy-grown films through the hybridization of the topological surface states with the hafnium (Hf) d-orbitals in the topmost layer of an underlying oxygen-deficient hafnium oxide (HfO2) substrate. The higher angular momentum of the d-orbitals of Hf is hybridized strongly by topological insulators, thereby enhancing the spin–orbit coupling and perturbing the topological surface states asymmetry in Bi2Se3. As the oxygen defect is cured or generated reversibly by external electric fields, our research facilitates the complete electrical control of the topological phases of topological insulators by controlling the defect density in the adjacent transition metal oxide. In addition, this mechanism can be applied in other related topological materials such as Weyl and Dirac semimetals in future endeavors to facilitate practical applications in unit-element devices for quantum computing and quantum communication.