Engineering Excitons through Polymorphism and Dimensional Confinement in Low-Dimensional Tellurium

Abstract

The interplay between dimensionality, band-edge electronic structure, and electron-hole interactions governs the optical response of low-dimensional tellurium, yet the microscopic origin of its excitonic behavior remains largely unexplored. Here, we investigate the quasiparticle, excitonic, and optical properties of two-dimensional tellurium polymorphs and one-dimensional helical nanowires using many-body GW and the Bethe--Salpeter equation. Our results reveal a strong dependence of the excitonic response on band-edge dispersion, crystal symmetry, and dimensional confinement. $\alpha$-tellurene exhibits comparatively weak and spatially extended electron-hole correlations, whereas the SOC-induced quasi-flat band-edge states of $\beta$-tellurene give rise to a strongly bound and anisotropic near-infrared exciton. Momentum-resolved BSE eigenvectors and real-space exciton wave functions directly reveal the contrasting localization and anisotropy of these excitonic states. Remarkably, hydrogen-passivated hexagonal tellurene, previously identified as a quantum spin Hall phase with $Z_2=1$, supports an even larger direct exciton binding energy of 0.51 eV together with a compact and nearly isotropic in-plane excitonic distribution. This demonstrates that strong electron-hole correlations are fully compatible with nontrivial band topology, while the binding strength and spatial character of the exciton remain strongly dependent on the underlying band-edge electronic structure and crystal symmetry. The one-dimensional helical nanowire represents the strong-confinement limit, exhibiting a direct high exciton binding energy and a pronounced shift of the optical response toward the ultraviolet.