Hybridized defects in solid-state materials as artificial molecules

Abstract

Two-dimensional materials can be crafted with structural precision approaching the atomic scale, enabling quantum defects-by-design. These defects are frequently described as "artificial atoms" and are emerging optically-addressable spin qubits. However, interactions and coupling of such artificial atoms with each other, in the presence of the lattice, is remarkably underexplored. Here we present the formation of "artificial molecules" in solids, introducing a new degree of freedom in control of quantum optoelectronic materials. Specifically, in monolayer hexagonal boron nitride as our model system, we observe configuration-and distance-dependent dissociation curves and hybridization of defect orbitals within the bandgap into bonding and antibonding orbitals, with splitting energies ranging from ∼ 10 meV to nearly 1 eV. We calculate the energetics of cis and trans out-of-plane defect pairs CHB-CHB against an in-plane defect pair CB-CB and find that in-plane defect pair interacts more strongly than out-of-plane pairs. We demonstrate an application of this chemical degree of freedom by varying the distance between CB and VN of CBVN and observe changes in the predicted peak absorption wavelength from the visible to the near-infrared spectral band. We envision leveraging this chemical degree of freedom of defect complexes to precisely control and tune defect properties towards engineering robust quantum memories and quantum emitters for quantum information science.