Silicon vacancies in SiC are of significant interest for quantum information and sensing due to their unusual combination of long spin coherence time, optical addressability, and room-temperature operation in an industrially-relevant semiconductor. We characterize the spin and optical properties of the V2 silicon vacancy in 4H-SiC for both single defects and ensembles. We also show that they can be deterministically placed with sub-micron precision using focused Li ion implantation. Low-temperature photoluminescence excitation spectroscopy of the spin-dependent optical transitions of single silicon vacancies reveals two sharp lines with linewidths near the radiative lifetime limit. These lines correspond to the m_s=±1/2 and m_s=±3/2 states of an S=3/2 spin system that can be optically initialized, coherently manipulated with RF pulses, and read out via spin-dependent photoluminescence. We measure the different properties of spins in the two bases, and compare them to theoretical models. To suppress the limiting effects of the nuclear spin bath, we grow isotopically purified SiC with a very low abundance of ²⁹Si and ¹³C. Our room temperature spin coherence measurements show orders-of-magnitude improvement of the coherence times in these materials. In particular, the inhomogeneous dephasing time T₂^* in the m_s=±1/2 basis shows a ~100x improvement, reaching 20 μs. We consider the prospects of this system for quantum sensing and as an efficient spin-photon interface for use in quantum networks.

This work was supported by the U.S. Office of Naval Research, the OSD Quantum Sciences and Engineering Program, the Defense Threat Reduction Agency, and the Center for Integrated Nanotechnologies, an Office of Science User Facility operated for the U.S. Department of Energy (DOE) Office of Science. Sandia National Laboratories is a multi-mission laboratory managed and operated by National Technology and Engineering Solutions of Sandia, LLC., a wholly owned subsidiary of Honeywell International, Inc., for the U.S. Department of Energy's National Nuclear Security Administration under contract DE-NA-0003525.