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Directly imaging structural dynamics involving hydrogen atoms by ultrafastdiffraction methods is complicated by their low scattering cross-sections. Herewe demonstrate that megaelectronvolt ultrafast electron diffraction issufficiently sensitive to follow hydrogen dynamics in isolated molecules. In astudy of the photodissociation of gas phase ammonia, we simultaneously observesignatures of the nuclear and corresponding electronic structure changesresulting from the dissociation dynamics in the time-dependent diffraction.Both assignments are confirmed by ab initio simulations of the photochemicaldynamics and the resulting diffraction observable. While the temporalresolution of the experiment is insufficient to resolve the dissociation intime, our results represent an important step towards the observation of protondynamics in real space and time.

Femtosecond electronic and hydrogen structural dynamics in ammonia imaged with ultrafast electron diffraction