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.

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Recent developments in attosecond technology led to table-top x-ray spectroscopy in the soft x-ray range, thus uniting the element-and statespecificity of core-level x-ray absorption spectroscopy with the time resolution to follow electronic dynamics in real-time. We describe recent work in attosecond technology and investigations into materials such as Si, SiO 2 , GaN, Al 2 O 3 , Ti, and TiO 2 , enabled by the convergence of these two capabilities. We showcase the state-of-the-art on isolated attosecond soft x-ray pulses for x-ray absorption near-edge spectroscopy to observe the 3d-state dynamics of the semi-metal TiS 2 with attosecond resolution at the Ti L-edge (460 eV). We describe how the element-and state-specificity at the transition metal L-edge of the quantum material allows us to unambiguously identify how and where the optical field influences charge carriers. This precision elucidates that the Ti:3d conduction band states are efficiently photo-doped to a density of 1.9 Â 10 21 cm À3 . The light-field induces coherent motion of intra-band carriers across 38% of the first Brillouin zone. Lastly, we describe the prospects with such unambiguous real-time observation of carrier dynamics in specific bonding or anti-bonding states and speculate that such capability will bring unprecedented opportunities toward an engineered approach for designer materials with pre-defined properties and efficiency. Examples are composites of semiconductors and insulators like Si, Ge, SiO 2 , GaN, BN, and quantum materials like graphene, transition metal dichalcogens, or high-Tc superconductors like NbN or LaBaCuO. Exiting are prospects to scrutinize canonical questions in multi-body physics, such as whether the electrons or lattice trigger phase transitions.

The identification of the cross-plane electric transport mechanisms in different resistance states of metal-oxide sandwich structures is essential for gaining insights into the mechanisms of resistive switching (RS). Here, we present a systematic study of cross-plane electric transport properties of Pr 0.67 Ca 0.33 MnO 3 (PCMO) thin films sandwiched by precious Pt metal electrodes. We observe three different transport regimes: ohmic, nonlinear and RS. The nonlinear regime is associated with colossal magneto-resistance (CMR) and colossal electro-resistance (CER) effects. In contrast to RS, the CMR and CER are volatile resistance effects which persist only during application of strong magnetic or electric fields and they are restricted to low temperatures. At low current densities, the device resistance is dominated by small polaron hopping transport of the PCMO film. At higher electric current densities near the switching threshold, the interface resistance starts to dominate and remarkably also exhibits thermally activated transport properties. Our studies also shed light onto the interplay of colossal resistance effects and RS: at low temperatures, RS can be only induced by reduction of the PCMO resistivity through CMR and CER. This clearly demonstrates the key role of the current density for controlling the amplitude of non-volatile resistive changes. Conversely, the CMR can be used as a probe for the switching induced changes in disorder and correlations. At small switching amplitudes, we observe slight changes in polaron activation