Probing quantum-coherent dynamics with free electrons

Recent advances in time-resolved cathodoluminescence have enabled ultrafast studies of single emitters in quantum materials with femtosecond temporal resolution. Here, we develop a quantum theory modeling the dynamics of free electrons interacting with quantum emitters in arbitrary initial states. Our analysis reveals that a free electron can induce transient coherent oscillations in the populations when the system is initially prepared in a coherent superposition of its states. Moreover, the electron energy spectrum exhibits a clear signature of the quantum coherence and sensitivity to the transition frequency of the emitter. These coherence effects manifest themselves as oscillations in the zero-loss peak of the spectral energy-loss probability. Our findings pave the way for characterization of quantum-coherent dynamics of individual quantum emitters by electron-probes.