Multiple-microwave-photon transition of nitrogen-vacancy centers in diamond

Multiple-microwave-photon transition is a nonlinear process involving the simultaneous absorption of multiple microwave photons to reach a higher energy state. This phenomenon enables microwave frequency conversion, a crucial technique for spin-wave devices, frequency synthesizers and communication devices. However, it has not been observed in nitrogen-vacancy (NV) centers in diamonds, which serve as a key quantum platform linking flying qubits, microwave photons, and solid-state spins. In this work, we first observed multiple-microwave-photon transitions in NV centers in diamonds, using optically detected magnetic resonance (ODMR) methods with a single laser and microwave beam. We demonstrate that microwave frequencies, effective g-factor, and angular momentum exhibit a 1/n scaling law, but the linewidth exhibits a 1/n^2 scaling law for n-photon transitions between the ground states. Additionally, we detect the hyperfine structure of the ground states and achieve coherent spin manipulation under multi-photon excitation. Our findings offer a novel approach for the precise manipulation of NV center spin states, advancing quantum sensing and quantum information.