Free-electron interaction with nonlinear optical states in microresonators

The short de Broglie wavelength and strong interaction empower free electrons to probe scattering and excitations in materials and resolve the structure of biomolecules. Recent advances in using nanophotonic structures to mediate bilinear electron-photon interaction have brought novel optical manipulation schemes to electron beams, enabling high space-time-energy resolution electron microscopy, quantum-coherent optical modulation, attosecond metrology and pulse generation, transverse electron wavefront shaping, dielectric laser acceleration, and electron-photon pair generation. However, photonic nanostructures also exhibit nonlinearities, which have to date not been exploited for electron-photon interactions. Here, we report the interaction of electrons with spontaneously generated Kerr nonlinear optical states inside a continuous-wave driven photonic chip-based microresonator. Optical parametric processes give rise to spatiotemporal pattern formation, or dissipative structures, corresponding to coherent or incoherent optical frequency combs. By coupling such microcombs in situ to electron beams, we demonstrate that different dissipative structures induce distinct fingerprints in the electron spectra and Ramsey-type interference patterns. In particular, using spontaneously formed femtosecond temporal solitons, we achieve ultrafast temporal gating of the electron beam without the necessity of a pulsed laser source or a pulsed electron source. Our work elucidates the interaction of free electrons with a variety of nonlinear dissipative states, demonstrates the ability to access solitons inside an electron microscope, and extends the use of microcombs to unexplored territories, with ramifications in novel ultrafast electron microscopy, light-matter interactions driven by on-chip temporal solitons, and ultra-high spatiotemporal resolution sampling of nonlinear optical dynamics and devices.