Ultrafast scanning electron microscopy with sub-micrometer optical pump resolution

Ultrafast scanning electron microscopy images carrier dynamics and carrier induced surface voltages using a laser pump electron probe scheme, potentially surpassing all-optical techniques in probe resolution and surface sensitivity. Current implementations have left a four order of magnitude gap between optical pump and electron probe resolution, which particularly hampers spatial resolution in the investigation of carrier induced local surface photovoltages. Here, we present a system capable of focusing the laser using an inverted optical microscope built into an ultrafast scanning electron microscopy setup to enable high numerical aperture pulsed optical excitation in conjunction with ultrafast electron beam probing. We demonstrate an order of magnitude improvement in optical pump resolution, bringing this to sub-micrometer length scales. We further show that temporal laser pump resolution can be maintained inside the scanning electron microscope by pre-compensating dispersion induced by the components required to bring the beam into the vacuum chamber and to a tight focus. We illustrate our approach using molybdenum disulfide, a two-dimensional transition metal dichalcogenide, where we measure ultrafast carrier relaxation rates and induced negative surface potentials between different flakes selected with the scanning electron microscope as well as on defined positions within a single flake.