Colossal Shift Currents in Band‐Inverted Bi Nanotubes Driven by the Interplay of Curvature and Spin‐Orbit Coupling

Abstract The concept of non‐trivial electronic structure combined with reduced dimensionality presents a promising strategy for advancing optical applications and energy harvesting technologies. Symmetry breaking in low dimensional system enables the emergence of non‐linear optical responses, which are greatly amplified by the singular points of band inversion. Here, using first‐principles calculations, the significant enhancement of the shift current in Bi nanotubes is investigated, driven by the combined effects of 1D geometry and non‐trivial band order. By rolling a 2D Bi monolayer, which exhibits a quantum spin Hall phase, into a 1D nanotube, an extraordinarily large shift current of 4.94 A·Å² V⁻² is generated, two orders of magnitude larger than the experimental values in WS₂ nanotubes. The enhancement of the shift current in Bi nanotubes is demonstrated and attributed to the state mixing induced by the interplay of strong spin‐orbit coupling, the curvature of the tube, and the non‐trivial band order of Bi nanotubes. The robustness of this enhanced shift current against various perturbations is also discussed, such as oxidation and doping. The novel approach integrating non‐trivial band order with reduced dimensionality sheds new light on advanced photovoltaic applications by harnessing both geometric advantages and exotic electronic structures for energy conversion.