Rabi oscillations and adiabatic passage of single electron spins in a diamond nitrogen vacancy center are demonstrated with two Raman-resonant optical pulses that are detuned from the respective dipole optical transitions. We show that the optical spin control is nuclear-spin selective and can be robust against rapid decoherence, including radiative decay and spectral diffusion, of the underlying optical transitions. A direct comparison between the Rabi oscillation and the adiabatic passage, along with a detailed theoretical analysis, provides significant physical insights into the connections and differences between these coherent spin processes and also elucidates the role of spectral diffusion in these processes. The optically driven coherent spin processes enable the use of nitrogen vacancy excited states to mediate coherent spin-phonon coupling, opening the door to combining optical control of both spin and mechanical degrees of freedom.

• Received 27 September 2013

DOI:https://doi.org/10.1103/PhysRevLett.112.116403