Phase-locked photon-electron interaction without a laser

Ultrafast photon-electron spectroscopy in electron microscopes commonly requires ultrafast laser setups. Photoemission from an engineered electron source is used to generate pulsed electrons, interacting with a sample excited by the laser pulse at a known time delay. Thus, developing an ultrafast electron microscope demands the exploitation of extrinsic laser excitations and complex synchronization schemes. Here we present an inverse approach to introduce internal radiation sources in an electron microscope based on cathodoluminescence spectroscopy. Our compact method is based on a sequential interaction of the electron beam with an electron-driven photon source and the investigated sample. Such a source in an electron microscope generates phase-locked photons that are mutually coherent with the near-field distribution of the swift electron. We confirm the mutual frequency and momentum-dependent correlation of the electron-driven photon source and sample radiation and determine a degree of mutual coherence of up to 27%. With this level of mutual coherence, we were able to perform spectral interferometry with an electron microscope. Our method has the advantage of being simple, compact and operating with continuous electron beams. It will open the door to local photon-electron correlation spectroscopy of quantum materials, single-photon systems and coherent exciton-polaritonic samples with nanometre resolution.