Theory of the CH$_\text{S}^-$ Defect in MoS$_2$ Confirming the Origin of the Quantum Emission

Abstract: Establishing the microscopic origin of localized emission in two-dimensional materials through consistent agreement between experiment and theory remains challenging. Recent STM/STS-STML measurements assigned an emission near 1.8 eV in monolayer MoS$<em>2$/hBN(2L)/graphene to the negatively charged CH$</em>\mathrm{S}<sup>{-}$ defect. However, a comprehensive theoretical description of this emitter is still lacking. Here, we develop such a description and systematically investigate the photophysical properties of CH$<em>\mathrm{S}<sup>{-}$ in monolayer MoS$_2$, two bilayer configurations, and a MoS$_2$/hBN heterostructure. The defect retains a similar local geometry and favors a singlet ground state in all four environments, whereas its electronic transition, zero-phonon line, electron-phonon coupling, radiative lifetime, and transition-dipole orientation depend strongly on the surrounding layers. The isolated-monolayer model exhibits substantial structural reorganization and produces a broad, dominant phonon sideband that is inconsistent with experiment. Adding an adjacent layer, either MoS$_2$ or hBN, substantially suppresses the phonon sideband, with only a minor dependence on the defect position in bilayer MoS$_2$. In particular, the MoS$_2$/hBN model yields a weak phonon sideband and closely reproduces the experimental photoluminescence lineshape. Our results thus provide the first theoretical agreement of CH$</em>\mathrm{S}<sup>{-}$ emission and further reveal the role of adjacent layers in determining the electronic, vibronic, and optical properties of the quantum emitters in two-dimensional materials.