Free-electron superfluorescence: collective optical dynamics at deep-subwavelength resolution

Long-range coherence and correlations between electrons in solids are the cornerstones for developing future quantum materials and devices. In 1954, Dicke described correlated spontaneous emission from closely packed quantum emitters, forming the theoretical basis of superradiance and superfluorescence. Since then, it has remained an open challenge to observe such phenomena with nanometer spatial resolution, precisely the important scale at which the collective correlations occur. Here, we report the first instance of free-electron-driven superfluorescence - superfluorescent cathodoluminescence - enabling us to excite and observe correlations at nanometer spatial scales. To exemplify this concept in our experiments, superlattices of lead halide perovskite quantum dots are excited by focused pulses of multiple free electrons. The electrons trigger superfluorescence: collective ultrafast emission observed at rates faster than both the lifetime and decoherence time. By controlling the area illuminated by the electron beam, we create a transition from a non-correlated spontaneous emission to a correlated superfluorescent emission. The observed signatures of superfluorescence are a reduction of the intrinsic emitter lifetime, a narrower linewidth, and a distinct redshift. We develop the theory of superfluorescent cathodoluminescence, which matches the results and highlights the unique features of electron-driven versus light-driven superfluorescence. Our observation and theory introduce a novel way to characterize coherence and correlations in quantum materials with nanometer spatial resolution, a key for future engineering of quantum devices.
Comment: 34 pages, 22 figures