Quantum Emitters at Telecommunication Wavelengths based on Carbon Defects in Transition Metal Dichalcogenides

Abstract

Low-dimensional materials have emerged as promising hosts for quantum emitters, whose emission typically arises from either strain-induced band bending or defect-induced two-level systems. Among these materials, transition metal dichalcogenide (TMD) monolayers have attracted particular attention; however, their performance is limited by strong photoluminescence (PL) quenching at room temperature. As TMDs transition from a direct to an indirect bandgap when moving from monolayers to multilayers, we herein propose a strategy to overcome this quenching limitation by exploiting the indirect bandgap of TMD bilayers in combination with a point defect doping. The indirect gap suppresses excitonic PL, while specific defects enable robust defect-mediated quantum emission. Using hybrid-functional density functional theory, we investigate substitutional carbon defects at chalcogen sites (S and Se) in WS2, WSe2, MoS2, and MoSe2 bilayers and comprehensively characterize their optical properties. Both neutral and singly negative charge states are found to be thermodynamically stable. Neutral defects exhibit singlet configurations with emission in the O- and C-band telecommunication windows, whereas negatively charged defects adopt doublet configurations featuring spin-selective transitions and near-infrared emission. The electron-phonon coupling strength, radiative lifetime, and dipole orientation are found to depend sensitively on both the host material and defect site, providing distinct fingerprints for experimental identification. Our findings, therefore, establish carbon-doped TMD bilayers as promising platforms for room-temperature defect-based quantum emitters operating at telecommunication wavelengths.