First-principles design of stable spin qubits in monolayer MoS₂ with elemental defect engineering

Abstract Quantum information science, encompassing technologies such as quantum computing, sensing, and communication, relies on the development and manipulation of quantum bits (qubits). Recently, two-dimensional (2D) materials—characterized by their atomic thinness and external controllability—have emerged as promising candidates for qubit fabrication and manipulation at room temperature. In this study, we propose that antisite defects (M X ) in 2D transition metal disulfides (TMDs) can serve as tunable quantum defects with controlled positioning. Using first-principles atomic structure simulations, we identify six thermodynamically stable neutral antisite defects (M X , where M = Mg, Ca, Sr, Ba, Zn, Cd; X = S) in monolayer 1H-MoS 2 . These defects exhibit potential as spin-defected qubits with stable triplet ground states. Additionally, we demonstrate that the reduction of the bandgap leads to significant fluctuations in the absorption coefficient within the low-energy range, resulting in the optical response within the desired telecommunication band, which is advantageous for quantum communication applications. The zero-phonon line associated with these qubits can serve as an effective identifier. This work presents the novel, tunable approach to exploiting defects in 2D materials, opening new possibilities for the development of qubit platforms in quantum information technology.