We demonstrate optomechanical quantum control of the internal electronic states of a diamond nitrogen-vacancy (NV) center in the resolved-sideband regime by coupling the NV to both optical fields and surface acoustic waves via a phonon-assisted optical transition and by taking advantage of the strong excited-state electron-phonon coupling of a NV center. Optomechanically driven Rabi oscillations as well as quantum interferences between the optomechanical sideband and the direct dipole-optical transitions are realized. These studies open the door to using resolved-sideband optomechanical coupling for quantum control of both the atomlike internal states and the motional states of a coupled NV-nanomechanical system, leading to the development of a solid-state analog of trapped ions.
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