A substitutional quantum defect in WS${}_2$ discovered by high-throughput computational screening and fabricated by site-selective STM manipulation

Abstract

Point defects in two-dimensional materials are of key interest for quantum information science. However, the space of possible defects is immense, making the identification of high-performance quantum defects extremely challenging. Here, we perform high-throughput (HT) first-principles computational screening to search for promising quantum defects within WS${}_2$, which present localized levels in the band gap that can lead to bright optical transitions in the visible or telecom regime. Our computed database spans more than 700 charged defects formed through substitution on the tungsten or sulfur site. We found that sulfur substitutions enable the most promising quantum defects. We computationally identify the neutral cobalt substitution to sulfur (Co${}_{\mathrm{S}}^0$) as very promising and fabricate it with scanning tunneling microscopy (STM). The Co${}_{\mathrm{S}}^0$ electronic structure measured by STM agrees with first principles and showcases an attractive new quantum defect. Our work shows how HT computational screening and novel defect synthesis routes can be combined to design new quantum defects.

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• Approximate Excited-State Potential Energy Surfaces for Defects in Solids
• First-principles computational methods for quantum defects in two-dimensional materials: A perspective
• NV-like Defects More Common Than Four-Leaf Clovers: A Perspective on High-Throughput Point Defect Data
• Computation of the expectation value of the spin operator ${\hat{S}}^2$ for the Spin-Flip Bethe-Salpeter Equation