Symmetry of the Hyperfine and Quadrupole Interactions of Boron Vacancies in a Hexagonal Boron Nitride

The concept of optically addressable spin states of deep-level defects in wide band gap materials is successfully applied for the development of quantum technologies. Recently discovered negatively charged boron vacancy defects (VB-) in hexagonal boron nitride (hBN) potentially allow a transfer of this concept onto atomic-thin layers due to the van der Waals nature of the defect host. Here, we experimentally explore all terms of the VB- spin Hamiltonian reflecting interactions with the three nearest nitrogen atoms by means of conventional electron spin resonance and high frequency (94 GHz) electron-nuclear double resonance. We establish symmetry, aniso-tropy, and principal values of the corresponding hyperfine interaction (HFI) and nuclear quadrupole interaction (NQI). The HFI can be expressed in the axially symmetric form as A perpendicular to = 45.5 +/- 0.9 MHz and A parallel to = 87 +/- 0.5 MHz, while the NQI is characterized by quadrupole coupling constant Cq = 1.96 +/- 0.05 MHz with slight rhombisity parameter eta = (Pxx - Pyy)/Pzz = -0.070 +/- 0.005. Utilizing a conventional approach based on a linear combination of atomic orbitals and HFI values measured here, we reveal that almost all spin density (approximate to 84%) of the VB- electron spin is localized on the three nearest nitrogen atoms. Our findings serve as valuable spectroscopic data and direct experimental demonstration of the VB- spin localization in a single two-dimensional BN layer.

Automated summary

The concept of optically addressable spin states of defects in wide band gap materials has been successfully applied in the development of quantum technologies. By studying the negatively charged boron vacancy defects (VB-) in hexagonal boron nitride (hBN), which has a van der Waals structure, the spin Hamiltonian and interactions with nearby nitrogen atoms have been experimentally explored. The results show a high localization of the VB- electron spin on the three nearest nitrogen atoms. These findings provide valuable spectroscopic data and demonstrate the spin localization in atomic-thin layers.