Since the discovery of electron-wave duality, electron scattering instrumentation has developed into a powerful array of techniques for revealing the atomic structure of matter. Beyond detecting local lattice variations in equilibrium structures with the highest possible spatial resolution, recent research efforts have been directed toward the long-sought-after dream of visualizing the dynamic evolution of matter in real time. The atomic behavior at ultrafast timescales carries critical information on phase transition and chemical reaction dynamics, the coupling of electronic and nuclear degrees of freedom in materials and molecules, and the correlation among structure, function, and previously hidden metastable or nonequilibrium states of matter. Ultrafast electron pulses play an essential role in this scientific endeavor, and their generation has been facilitated by rapid technical advances in both ultrafast laser and particle accelerator technologies. This review presents a summary of the noteworthy developments in this field in the last few decades. The physics and technology of ultrafast electron beams is presented with an emphasis on the figures of merit most relevant for ultrafast electron diffraction experiments. Recent developments in the generation, manipulation, and characterization of ultrashort electron beams aimed at improving the combined spatiotemporal resolution of these measurements are discussed. The fundamentals of electron scattering from atomic matter and the theoretical frameworks for retrieving dynamic structural information from solid-state and gas-phase samples is described. Essential experimental techniques and several landmark works that have applied these approaches are also highlighted to demonstrate the widening applicability of these methods. Ultrafast electron probes with ever-improving capabilities, combined with other complementary photon-based or spectroscopic approaches, hold tremendous potential for revolutionizing our ability to observe and understand energy and matter at atomic scales.

For 40 years, uniformly filled ellipsoidal beam distributions have been studied theoretically, as they hold the promise of generating self-fields linear in the coordinate offset in all three directions. Recently, a scheme for producing such distributions, based on the strong longitudinal expansion of an initially very short beam under its own space-charge forces, has been proposed. In this Letter we present the experimental demonstration of this scheme, obtained by illuminating the cathode in a rf photogun with an ultrashort laser pulse ($\sim 35\mathrm{fs}$ rms) with an appropriate transverse profile. The resulting 4 MeV beam spatiotemporal ($x,t$) distribution is imaged using a rf deflecting cavity with 50 fs resolution. A temporal asymmetry in the ellipsoidal profile, due to image charge effects at the photocathode, is observed at higher charge operation. This distortion is also found to degrade the transverse beam quality.

Pushing the limits in temporal resolution for transmission electron microscopy (TEM) requires a revolutionary change in the electron source technology. In this paper, we study the possibility of employing a radio-frequency photoinjector as the electron source for a time-resolved TEM. By raising the beam energy to the relativistic regime, we minimize the space-charge effects which otherwise limit the spatiotemporal resolution of the instrument. Analysis and optimization of the system taking into account the achievable beam brightness, electron flux on the sample, chromatic and spherical aberration of the electron optic system, and space-charge effects in image formation are presented and supported by detailed numerical modeling. The results demonstrate the feasibility of 10-nm–10-ps spatiotemporal resolution single-shot MeV TEM.

We report the experimental demonstration of time-resolved relativistic electron diffraction. Single shot diffraction patterns from a single crystal gold sample were recorded using ultrashort 3.5 MeV electron bunches from a radio frequency photoinjector. By scanning the pump pulse time-delay, we studied the Bragg peaks amplitude change due to the laser-induced melting of the sample. The observed time scale matches the one predicted using a simple two temperature model of the heating of the thin foil. Time-resolved relativistic electron diffraction using megaelectronvolt electron beams with ${10}^7$ particles in 100 fs bunch length opens exciting possibilities in ultrafast structural dynamics.

We experimentally investigate surface-plasmon assisted photoemission to enhance the efficiency of metallic photocathodes for high-brightness electron sources. A nanohole array-based copper surface was designed to exhibit a plasmonic response at 800 nm, fabricated using the focused ion beam milling technique, optically characterized and tested as a photocathode in a high power radio frequency photoinjector. Because of the larger absorption and localization of the optical field intensity, the charge yield observed under ultrashort laser pulse illumination is increased by more than 100 times compared to a flat surface. We also present the first beam characterization results (intrinsic emittance and bunch length) from a nanostructured photocathode.

Single shot diffraction patterns using a 250-fs-long electron beam have been obtained at the UCLA Pegasus laboratory. High quality images with spatial resolution sufficient to distinguish closely spaced peaks in the Debye–Scherrer ring pattern have been recorded by scattering the 1.6 pC 3.5 MeV electron beam generated in the rf photoinjector off a 100-nm-thick Au foil. Dark current and high emittance particles are removed from the beam before sending it onto the diffraction target using a 1 mm diameter collimating hole. These results open the door to the study of irreversible phase transformations by single shot MeV electron diffraction.