Precise coherent control of the individual electronic spins associated with atom-like impurities in the solid state is essential for applications in quantum information processing and quantum metrology. We demonstrate all-optical initialization, fast coherent manipulation, and readout of the electronic spin of the negatively charged nitrogen-vacancy (NV − ) center in diamond at T∼7K. We then present the observation of a novel double-dark resonance in the spectroscopy of an individual NV center. These techniques open the door for new applications ranging from robust manipulation of spin states using geometric quantum gates to quantum sensing and information processing.
PACS numbers:The negatively charged nitrogen-vacancy (NV − ) center in diamond is an atom-like impurity in the solid state that combines a long lived spin-triplet ground state with coherent optical transitions. A number of recent experiments and novel applications have been enabled by the use of a combination of visible frequency lasers to address the electronic states and microwave manipulation to address the spin degree of freedom [1][2][3][4][5]. While techniques for microwave spin manipulation of NV centers are well established, a number of new potential applications could be enabled by controlling the ground state spin sublevels using optical Raman transitions as is done with isolated neutral atoms and ions. For example, the use of multiple Raman transitions between four-level tripod systems was proposed for realization of robust geometrical quantum gates [6,7]. In addition, optical manipulation offers possibilities for improving NV-based metrology applications, for example by providing access to forbidden transitions between spin sublevels that are more sensitive to magnetic fields [8,9]. Moreover, all-optical manipulation techniques are important for the development of integrated nanophotonic systems for diamond-based scalable quantum optical devices and quantum networks [10][11][12]. In these devices, microwave structures on the diamond substrate are often incompatible with the fabrication process for the nanophotonic devices, while the use of external microwave source defeat the scalability of on-chip photonic devices. The complex level structure and selection rules of the NV center's optical transitions offer a rich and flexible set of possibilities for coherent all-optical control of all three spin sublevels. Past experiments have demonstrated optical spin manipulation under a large magnetic field or two-photon Rabi oscillations and stimulated Raman adiabatic passage (STIRAP) on microsecond timescales [13][14][15].In this Letter, we demonstrate complete all-optical coherent manipulation of the NV spin states. Importantly, initialization and readout of the spin states are also performed all-optically, providing a full set of experimental techniques that eliminates the need for microwave addressing. In addition, we report the first observations of nearly degenerate dark states associated with a doubledark resonance in a single quantum emit...