We present the development of the first ultrafast transmission electron microscope (UTEM) driven by localized photoemission from a field emitter cathode. We describe the implementation of the instrument, the photoemitter concept and the quantitative electron beam parameters achieved. Establishing a new source for ultrafast TEM, the Göttingen UTEM employs nano-localized linear photoemission from a Schottky emitter, which enables operation with freely tunable temporal structure, from continuous wave to femtosecond pulsed mode. Using this emission mechanism, we achieve record pulse properties in ultrafast electron microscopy of 9Å focused beam diameter, 200fs pulse duration and 0.6eV energy width. We illustrate the possibility to conduct ultrafast imaging, diffraction, holography and spectroscopy with this instrument and also discuss opportunities to harness quantum coherent interactions between intense laser fields and free-electron beams.

Understanding microscopic processes in materials and devices that can be switched by light requires experimental access to dynamics on nanometer length and femtosecond time scales. Here, we introduce ultrafast dark-field electron microscopy to map the order parameter across a structural phase transition. We use ultrashort laser pulses to locally excite a 1T-TaS2 (1T-polytype of tantalum disulfide) thin film and image the transient state of the specimen by ultrashort electron pulses. A tailored dark-field aperture array allows us to track the evolution of charge-density wave domains in the material with simultaneous femtosecond temporal and 5-nanometer spatial resolution, elucidating relaxation pathways and domain wall dynamics. The distinctive benefits of selective contrast enhancement will inspire future beam-shaping technology in ultrafast transmission electron microscopy.

Tip-based photoemission electron sources offer unique properties for ultrafast imaging, diffraction, and spectroscopy experiments with highly coherent few-electron pulses. Extending this approach to increased bunch-charges requires a comprehensive experimental study on Coulomb interactions in nanoscale electron pulses and their impact on beam quality. For a laser-driven Schottky field emitter, we assess the transverse and longitudinal electron pulse properties in an ultrafast transmission electron microscope at a high photoemission current density. A quantitative characterization of electron beam emittance, pulse duration, spectral bandwidth, and chirp is performed. Due to the cathode geometry, Coulomb interactions in the pulse predominantly occur in the direct vicinity to the tip apex, resulting in a well-defined pulse chirp and limited emittance growth. Strategies for optimizing electron source parameters are identified, enabling advanced ultrafast transmission electron microscopy approaches, such as phase-resolved imaging and holography.

Strategies to optically control and modify physical material properties have a strong impact in current and future technologies. The underlying dynamical processes generally take place on femto-to picosecond timescales, a regime accessible by a wide variety of stroboscopic pump/probe approaches. When applied to actual devices, however, functionality usually also arises from nanoscale structuring or an interplay of different materials. This calls for experimental approaches capturing optically induced dynamics in terms of a spatially dependent order parameter.

While correlated electrons are at the heart of many phenomena in condensed matter, as well as atomic and molecular physics, Coulomb interactions in free-electron beams are generally considered detrimental. Here, we demonstrate the generation of Coulomb-correlated pair, triple and quadruple states of free electrons by femtosecond photoemission from a nanoscale field emitter inside a transmission electron microscope. Event-based electron spectroscopy allows the spatial and spectral characterization of the electron ensemble emitted by each laser pulse. We identify distinctive energy and momentum correlations arising from acceleration-enhanced interparticle energy exchange, revealing strong few-body Coulomb interactions at an energy scale of 2 eV. State-sorted beam caustics show a discrete increase in virtual source size and longitudinal source shift for few-electron states, associated with transverse momentum correlations. We observe field-controllable electron antibunching, attributed primarily to transverse Coulomb deflection. The pronounced spatial and spectral characteristics of these electron number states allow filtering schemes that control the statistical distribution of the pulse charge. In this way, the fraction of specific few-electron states can be actively suppressed or enhanced, facilitating the preparation of highly non-Poissonian electron beams for microscopy and lithography, including future heralding schemes and correlated multi-electron probing.

The tunability of materials properties by light promises a wealth of future applications in energy conversion and information technology. Strongly correlated materials such as transition metal dichalcogenides offer optical control of electronic phases, charge ordering and interlayer correlations by photodoping. Here, we find the emergence of a transient hexatic state during the laser-induced transformation between two charge-density wave phases in a thin-film transition metal dichalcogenide, 1T-type tantalum disulfide (1T-TaS2). Introducing tilt-series ultrafast nanobeam electron diffraction, we reconstruct charge-density wave rocking curves at high momentum resolution. An intermittent suppression of three-dimensional structural correlations promotes a loss of in-plane translational order caused by a high density of unbound topological defects, characteristic of a hexatic intermediate. Our results demonstrate the merit of tomographic ultrafast structural probing in tracing coupled order parameters, heralding universal nanoscale access to laser-induced dimensionality control in functional heterostructures and devices.

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We demonstrate the generation and optical control of ultrashort high-coherence electron pulses. The free-electron quantum state is phase-modulated in the longitudinal and transverse dimensions, and the formation of attosecond electron pulse trains is quantitatively probed.