High-Throughput Search for Triplet Point Defects with Narrow Emission Lines in 2D Materials

We employ a first-principles computational workflow to screen for optically accessible, high-spin point defects in wide band gap, two-dimensional (2D) crystals. Starting from an initial set of 5388 point defects, comprising both native and extrinsic, single and double defects in ten previously synthesized 2D host materials, we identify 596 defects with a triplet ground state. For these defects, we calculate the defect formation energy, hyperfine (HF) coupling, and zero-field splitting (ZFS) tensors. For 39 triplet transitions exhibiting particularly low Huang-Rhys factors, we calculate the full photoluminescence (PL) spectrum. Our approach reveals many spin defects with narrow PL line shapes and emission frequencies covering a broad spectral range. Most of the defects are hosted in hexagonal BN (hBN), which we ascribe to its high stiffness, but some are also found in MgI₂, MoS₂, MgBr₂ and CaI₂. As specific examples, we propose the defects v_SMo_S⁰ and Ni_SMo_S⁰ in MoS₂ as interesting candidates with potential applications to magnetic field sensors and quantum information technology.