Optically detected magnetic resonance in the neutral silicon vacancy center in diamond via bound exciton states.

Neutral silicon vacancy (SiV0) centers in diamond are promising candidates for quantum networks because they feature both excellent optical properties and long spin coherence times. However, spin-dependent fluorescence in such defects has been elusive. In contrast to nitrogen vacancy (NV) centers, the high Debye-Waller factor and correspondingly smaller phonon sideband make off-resonant spin polarization challenging, and optically detected magnetic resonance (ODMR) utilizing the zero phonon line is complicated by limited emission in the phonon sideband and poor understanding of the excited state fine structure. Here we report the realization of ODMR and coherent control of the SiV0 center, enabled by efficient optical spin polarization via higher-lying excited states. We assign these states to be bound exciton states of SiV0 by combining group theory and giant supercell density functional theory (DFT) calculations. These higher-lying states enable efficient optical excitation and spin polarization for SiV0 and provide new possibilities for controlling SiV0 as well as other similar defect systems.