Room temperature coherent control of a single solid-state spin under anti-Stokes excitation

Single-spin qubits in solid-state materials are important fundamental platforms for quantum information applications. Traditionally, coherent control of solid-state defects is realized under Stokes excitation. Little is known about the coherent control of a single defect spin under anti-Stokes excitation. In this work, we experimentally verify that the mechanism of anti-Stokes excitation of the divacancy in silicon carbide is a phonon-assisted single-photon absorption process and provide the confocal microscopy anti-Stokes photoluminescence scanning image of an isolated single divacancy. Moreover, the optically detected magnetic resonance measurement and coherent control of the single divacancy spin under anti-Stokes excitation are realized at room temperature. We further reveal that the spin readout contrast under anti-Stokes excitation is more robust than that under Stokes excitation at elevated temperatures. Our work establishes a nontraditional protocol for the optical addressing and coherent control of single-spin qubits and expands the boundary of quantum information technology.