Twist-engineering of a robust Quantum Spin Hall phase in $β$-/flat bismuthene bilayer from first principles

Abstract

Twist-engineering of topological phases in two-dimensional materials offers a powerful route to modulate electronic structure beyond conventional strain or chemical control. In particular, group 15 (pnictogens) monolayers such as bismuthene provide an ideal platform due to their strong intrinsic spin-orbit coupling (SOC) and robust topological character. Here, we investigate a previously unexplored heterostructure consisting of a $β$-bismuthene monolayer rotated by 30$^\circ$ on a planar bismuthene layer stabilized on a SiC(0001) substrate. Using first-principles calculations, we demonstrate that this specific rotational alignment induces a unique interlayer orbital hybridization which, combined with the strong SOC and the naturally broken inversion symmetry, gives rise to a pronounced Rashba spin-splitting, absent in the isolated monolayers. The topological nature of the system is confirmed through the calculation of the Z2 topological invariant and Spin Hall Conductivity (SHC), revealing a robust Quantum Spin Hall (QSH) phase with an enhanced topological response compared to the individual layers. Furthermore, we explore the chemical tunability of this system via Sb substitution, showing that the gradual reduction of SOC systematically narrows the band gap while preserving the non-trivial topology. Our results establish large-angle twisted group 15 heterostructures as a versatile platform for engineering spin-orbit-driven phenomena and advancing topological spintronics.