Spin-optical dynamics and quantum efficiency of single V1 center in silicon carbide (2203.08177v2)

Abstract: Color centers in silicon carbide are emerging candidates for distributed spin-based quantum applications due to the scalability of host materials and the demonstration of integration into nanophotonic resonators. Recently, silicon vacancy centers in silicon carbide have been identified as a promising system with excellent spin and optical properties. Here, we in-depth study the spin-optical dynamics of single silicon vacancy center at hexagonal lattice sites, namely V1, in 4H-polytype silicon carbide. By utilizing resonant and above-resonant sub-lifetime pulsed excitation, we determine spin-dependent excited-state lifetimes and intersystem-crossing rates. Our approach to inferring the intersystem-crossing rates is based on all-optical pulsed initialization and readout scheme, and is applicable to spin-active color centers with similar dynamics models. In addition, the optical transition dipole strength and the quantum efficiency of V1 defect are evaluated based on coherent optical Rabi measurement and local-field calibration employing electric-field simulation. The measured rates well explain the results of spin-state polarization dynamics, and we further discuss the altered photoemission dynamics in resonant enhancement structures such as radiative lifetime shortening and Purcell enhancement. By providing a thorough description of V1 center's spin-optical dynamics, our work provides deep understanding of the system which guides implementations of scalable quantum applications based on silicon vacancy centers in silicon carbide.