Isolated nuclear spins offer a promising building block for quantum information processing systems, but their weak interactions often impede preparation, control, and detection. Hyperfine coupling to a proximal electronic spin can enhance each of these processes. Using the electronic spin of the nitrogen-vacancy center as an intermediary, we demonstrate robust initialization, single-qubit manipulation, and direct optical readout of 13C, 15N, and 14N nuclear spins in diamond. These results pave the way for nitrogen nuclear spin based quantum information architectures in diamond

Magnetic resonance techniques provide a powerful tool for controlling spin systems, with applications ranging from quantum information processing to medical imaging. Nevertheless, the behavior of a spin system under strong excitation remains a rich dynamical problem. In this paper, we examine spin resonance of the nitrogen-vacancy center in diamond under conditions outside the regime where the usual rotating wave approximation applies, focusing on effects of multifrequency excitation and excitation with orientation parallel to the spin quantization axis. Strong-field phenomena such as multiphoton transitions and coherent destruction of tunneling are observed in the spectra and analyzed via numerical and analytic theory. In addition to illustrating the response of a spin system to strong multifrequency excitation, these observations may inform techniques for manipulating electron-nuclear spin quantum registers.