Kinetics-Driven Selective Stoichiometric Shift and Structural Asymmetry in $Bi_4Te_3$ Nanostructures for Hybrid Quantum Architectures

Abstract

Advances in hybrid quantum architectures hinge on topological materials that can be synthesized with precise stoichiometric and structural control at the nanoscale. While $Bi_4Te_3$ is a promising candidate due to its dual topological phases, acting as both a strong topological insulator and a topological crystalline insulator, high-quality growth remains challenging due to a narrow stoichiometric window and high sensitivity to surface kinetics. Here, we establish a reproducible molecular beam epitaxy (MBE) process to produce stoichiometric, twin-free $Bi_4Te_3$ thin films with ultra-smooth surfaces and atomically sharp van der Waals stacks. By employing selective area epitaxy (SAE), we realize laterally confined $Bi_4Te_3$ nanostructures that exhibit a feature-dependent stoichiometric deviation. This phenomenon, which we term the selective stoichiometric shift, arises from the unequal lateral diffusion of Bi and Te adatoms, revealing a direct coupling between adatom kinetics and nanoscale compositional stability. Atomic-resolution imaging further uncovers asymmetric van der Waals gaps within the stacking sequence, identifying an intrinsic structural asymmetry between the quintuple and bilayer units. These findings provide fundamental insights into the crystallization of Bi_4Te_3$ and demonstrate a scalable route for integrating functional topological materials into next-generation superconducting hybrid quantum circuits.