Identification of an Oxygen Defect in Hexagonal Boron Nitride

Paramagnetic fluorescent defects in two-dimensional hexagonal boron nitride (hBN) are promising building blocks for quantum information processing. Although numerous defect-related single-photon sources and a few quantum bits have been found, except for the boron vacancy, their identification is still elusive. Here, we demonstrate that the comparison of experimental and first-principles simulated electron paramagnetic resonance (EPR) spectra is a powerful tool for defect identification in hBN, and first-principles modeling is inevitable in this process as a result of the dense nuclear spin environment of hBN. In particular, a recently observed EPR center is associated with the negatively charged oxygen vacancy complex by means of the many-body perturbation theory method on top of hybrid density functional calculations. To our surprise, the negatively charged oxygen vacancy complex produces a coherent emission around 2 eV with a well-reproducing previously recorded photoluminescence spectrum of some quantum emitters, according to our calculations.