Theoretical Investigation of Twist-Angle-Dependent Photoelectric Properties in Twisted Bilayer WSe2

The twist angle serves as a geometric tuning parameter in two-dimensional layered materials, enabling modulation of interlayer coupling and band structures without altering the chemical composition. In this work, six commensurate twisted bilayer WSe2 configurations with rotation angles of 0°, 9.4°, 13.14°, 21.9°, 27.8°, and 60° were systematically investigated using first-principles density functional theory. Structural optimization, together with calculations of electronic structures, density of states, charge redistribution, effective masses, and optical properties, was performed. The results show that AA (0°) and 2H (60°) stackings exhibit the largest and smallest interlayer separations, respectively, whereas intermediate twist angles yield similar average spacings but distinct local stacking registries. All configurations remain indirect-gap semiconductors, with the valence band maximum located at K and the conduction band minimum near the Q point along the K–Γ path. The band gap increases from 1.450 eV at 0° to 1.579 eV at 27.8°, before decreasing to 1.333 eV at 60°, indicating strong twist-angle modulation of interlayer coupling. Density-of-states analysis shows that the valence-band edge mainly originates from Se-p and W-d hybridized states, whereas the conduction-band edge is dominated by W-d states, with intermediate angles exhibiting enhanced band folding and localization features. Charge-density analyses further reveal notable interfacial charge redistribution, which is most pronounced at 9.4°. Optical responses in the in-plane directions are nearly identical and significantly stronger than those along the out-of-plane direction. Optical absorption mainly occurs in the ultraviolet region, with band-edge features appearing in the near-infrared range. Intermediate twist angles exhibit broader dielectric responses in the visible region and extended long-wavelength tails, indicating enhanced interband transition channels. These results demonstrate that twist-angle engineering enables effective tuning of electronic and optical properties in bilayer WSe2, providing theoretical guidance for the design of tunable optoelectronic devices.