ArXiv · 2026
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 MoS₂/hBN(2L)/graphene to the negatively charged CHS⁻ 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 CHS⁻ in monolayer MoS₂, two bilayer configurations, and a MoS₂/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 MoS₂ or hBN, substantially suppresses the phonon sideband, with only a minor dependence on the defect position in bilayer MoS₂. In particular, the MoS₂/hBN model yields a weak phonon sideband and closely reproduces the experimental photoluminescence lineshape. Our results thus provide the first theoretical agreement of CHS⁻ 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.
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