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The use of relativistic electron pulses at kinetic energies in the megaelectronvolt (MeV) range has revolutionized investigations of ultrafast structural dynamics in recent years. This chapter reviews the technical developments leading to their application in ultrafast electron diffraction (UED) experiments. It also examines the specific properties of MeV electrons that make them ideal for such studies. We describe the instrumentation and methodology for MeV-UED in the gas phase, liquid phase, and solid state. We use the UED user facility at the SLAC National Accelerator Laboratory as an example to highlight recent experimental results from these research areas.

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