Hybridized defects in solid-state materials as artificial molecules

TL;DR

This paper demonstrates the creation of artificial molecules in 2D materials, revealing how defect interactions can be controlled to tune quantum properties for potential quantum information applications.

Contribution

It introduces the concept of defect molecules in solid-state materials, showing how defect interactions can be engineered to control quantum optoelectronic properties.

Findings

Observation of configuration- and distance-dependent defect hybridization.

Splitting energies of defect orbitals range from ~10 meV to nearly 1 eV.

Variation of defect pair distances alters optical absorption wavelengths.

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 $\sim$ 10 meV to nearly 1 eV. We calculate the energetics of $cis$ and $trans$ out-of-plane defect pairs CH$_\textrm{B}$-CH$_\textrm{B}$ against an in-plane defect pair C$_\textrm{B}$-C$_\textrm{B}$ 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 C$_\textrm{B}$ and V$_\textrm{N}$ of C$_\textrm{B}$V$_\textrm{N}$ 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.