Excited-state spin-resonance spectroscopy of VB− defect centers in hexagonal boron nitride

The recently discovered spin-active boron vacancy (V B ) defect center in hexagonal boron nitride (hBN) has high contrast optically-detected magnetic resonance (ODMR) at roomtemperature, 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 groundstate. 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 groundand 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 from D3h to C2v. Additionally, the excited-state ODMR has strong temperature dependence of both contrast and transverse anisotropy splitting, enabling promising avenues for quantum sensing. https://doi.org/10.1038/s41467-022-30772-z OPEN

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