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Ultrafast transmission electron microscopy (UTEM) has emerged as a versatile technique for the time-resolved imaging of nanoscale dynamics on timescales down to few-hundred attoseconds but the temporal and spatial resolutions are still limited by the coherence properties of pulsed electron sources. Here, we report the development of a novel laser-driven linear cold-field electron emitter integrated in a state-of-the-art UTEM system. Illuminating the sharp tungsten emitter tip with a UV light pulse generates ultrashort femtosecond electron pulses of 220 fs pulse duration, with energy widths as low as 360 meV. The photoelectron emitter demonstrates exceptional spatial coherence, achieving focal spot sizes down to 2 $\mathring {\mathrm A}$ and a peak normalized brightness exceeding 6.7 $\times 10^{13}$ A/m$^2$sr. With an order-of-magnitude improvement compared to previously employed laser-driven Schottky field emitters, the present development opens up the field of ultrafast atomic-scale electron probing., Comment: 20 pages, Manuscript + Supporting Information

The phase-resolved imaging of confined light fields by homodyne detection is a cornerstone of metrology in nano-optics and photonics, but its application in electron microscopy has been limited so far. Here, we report the mapping of optical modes in a waveguide structure by illumination with femtosecond light pulses in a continuous-beam transmission electron microscope. Multi-photon photoemission results in a remanent charging pattern which we image by Lorentz microscopy. The resulting image contrast is linked to the intensity distribution of the standing light wave and quantitatively described within an analytical model. The robustness of the approach is showcased in a wider parameter range and more complex sample geometries including micro- and nanostructures. We discuss further applications of light-interference-based charging for electron microscopy with in-situ optical excitation, laying the foundation for advanced measurement schemes for the phase-resolved imaging of propagating light fields., Comment: 32 pages, Manuscript + Supporting Information

Surface charging is a phenomenon ubiquitously observable in in-situ transmission electron microscopy of non-conducting specimens as a result of electron beam/sample interactions or optical stimuli and often limits the achievable image stability and spatial or spectral resolution. Here, we report on the electron-optical imaging of surface charging on a nanostructured surface following femtosecond-multiphoton photoemission. By quantitatively extracting the light-induced electrostatic potential and studying the charging dynamics on the relevant timescales, we gain insights into the details of the multi-photon photoemission process in the presence of a background field. We study the interaction of the charge distribution with the high-energy electron beam and secondary electrons and propose a simple model to describe the interplay of electron- and light-induced processes. In addition, we demonstrate how to mitigate sample charging by simultaneous optical illumination of the sample., Comment: 29 pages; Manuscript with 4 figures and Supporting Information with 1 additional figure and 4 videos