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Since the notion of topological insulator (TI) was envisioned in late 2000s, topology has become a new paradigm in condensed matter physics. Realization of topology as a generic property of materials has led to numerous predictions of topological effects. Although most of the classical topological effects, directly resulting from the presence of the spin-momentum-locked topological surface states (TSS), were experimentally confirmed soon after the theoretical prediction of TIs, many topological quantum effects remained elusive for a long while. It turns out that native defects, particularly interfacial defects, have been the main culprit behind this impasse. Even after quantum regime is achieved for the bulk states, TSS still tends to remain in the classical regime due to high density of interfacial defects, which frequently donate mobile carriers due to the very nature of the topologically-protected surface states. However, with several defect engineering schemes that suppress these effects, a series of topological quantum effects have emerged including quantum anomalous Hall effect, quantum Hall effect, quantized Faraday/Kerr rotations, topological quantum phase transitions, axion insulating state, zeroth-Landau level state, etc. Here, we review how these defect engineering schemes have allowed topological surface states to pull out of the murky classical regime and reveal their elusive quantum signatures, over the past decade. 

Abstract The interface between 2D topological Dirac states and ans‐wave superconductor is expected to support Majorana‐bound states (MBS) that can be used for quantum computing applications. Realizing these novel states of matter and their applications requires control over superconductivity and spin‐orbit coupling to achieve spin‐momentum‐locked topological interface states (TIS) which are simultaneously superconducting. While signatures of MBS have been observed in the magnetic vortex cores of bulk FeTe_0.55Se_0.45, inhomogeneity and disorder from doping make these signatures unclear and inconsistent between vortices. Here superconductivity is reported in monolayer (ML) FeTe_1–ySe_y(Fe(Te,Se)) grown on Bi₂Te₃by molecular beam epitaxy (MBE). Spin and angle‐resolved photoemission spectroscopy (SARPES) directly resolve the interfacial spin and electronic structure of Fe(Te,Se)/Bi₂Te₃heterostructures. Fory = 0.25, the Fe(Te,Se) electronic structure is found to overlap with the Bi₂Te₃TIS and the desired spin‐momentum locking is not observed. In contrast, fory = 0.1, reduced inhomogeneity measured by scanning tunneling microscopy (STM) and a smaller Fe(Te,Se) Fermi surface with clear spin‐momentum locking in the topological states are found. Hence, it is demonstrated that the Fe(Te,Se)/Bi₂Te₃system is a highly tunable platform for realizing MBS where reduced doping can improve characteristics important for Majorana interrogation and potential applications.