Quasiparticle electronic structure and excitonic effects in Janus CrSO monolayers are investigated by many-body calculations within first principles
Phys. Rev. B 114, 245125 – Published 19 October, 2026
DOI: https://doi.org/10.1103/fmdw-844l
Abstract
Transition-metal chalcogenide monolayers, with their intrinsic out-of-plane asymmetry and strong spin-orbit coupling, provide an exceptional platform for emergent excitonic and valley-dependent optoelectronic phenomena. Here, we present a comprehensive many-body investigation of the electronic structure and excitonic properties of the CrSO Janus monolayer using density functional theory, quasiparticle calculations, and the spinorial Bethe-Salpeter equation. The quasiparticle band structure reveals an indirect fundamental gap of 0.94 eV and a direct optical gap of 1.97 eV, highlighting pronounced many-body renormalization effects. Spinorial calculations uncover a strongly correlated excitonic manifold composed of both dark and bright excitons with large binding energies. In particular, a spin-forbidden dark exciton emerges at , followed by a spin-allowed bright exciton at , yielding a sizable spin-orbit-induced dark-bright splitting of 119 meV. Analysis of the excitonic spin texture reveals a dominant triplet character for the dark state and a mixed singlet-triplet configuration for the bright exciton. The reciprocal-space exciton wave functions exhibit strong valley localization around the and valleys, demonstrating the valley-selective nature of the optical transitions. Furthermore, electron-hole interactions dramatically reshape the optical response, enhancing the absorption intensity by up to 7.4 times relative to the independent-particle picture and generating broadband optical activity spanning 1.77–3.10 eV across the visible and near-ultraviolet regions. These results establish the CrSO Janus monolayer as a promising excitonic material for next-generation valleytronic, optoelectronic, and visible-light-driven energy-conversion technologies.