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Excited-state spin-resonance spectroscopy of V$${}_{{{{{{{{\rm{B}}}}}}}}}^{-}$$ defect centers in hexagonal boron nitride

https://doi.org/10.1038/s41467-022-30772-z

Mathur, Nikhil ; Mukherjee, Arunabh ; Gao, Xingyu ; Luo, Jialun ; McCullian, Brendan A. ; Li, Tongcang ; Vamivakas, A. Nick ; Fuchs, Gregory D. ( June 2022 , Nature Communications)

Abstract
The recently discovered spin-active boron vacancy (V$${}_{{{{{{{{\rm{B}}}}}}}}}^{-}$$ $_{B}^{-}$ ) defect center in hexagonal boron nitride (hBN) has high contrast optically-detected magnetic resonance (ODMR) at room-temperature, with a spin-triplet ground-state that shows promise as a quantum sensor. Here we report temperature-dependent ODMR spectroscopy to probe spin within the orbital excited-state. Our experiments determine the excited-state spin Hamiltonian, including a room-temperature zero-field splitting of 2.1 GHz and a g-factor similar to that of the ground-state. We confirm that the resonance is associated with spin rotation in the excited-state using pulsed ODMR measurements, and we observe Zeeman-mediated level anti-crossings in both the orbital ground- and excited-state. Our observation of a single set of excited-state spin-triplet resonance from 10 to 300 K is suggestive of symmetry-lowering of the defect system fromD_3htoC_2v. Additionally, the excited-state ODMR has strong temperature dependence of both contrast and transverse anisotropy splitting, enabling promising avenues for quantum sensing.

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