A key challenge in ultrafast science has been to directly track the coupled motions of electrons and nuclei in real space and real time. This Letter presents a significant step toward this goal by demonstrating the feasibility of time-resolved real-space tracking of valence electron and hydrogen dynamics during the photodissociation of ammonia (${\mathrm{NH}}_3$) using MeV ultrafast electron diffraction. It is demonstrated that the enhanced temporal resolution, in conjunction with the analysis of the charge-pair distribution function, enables the disentanglement of the correlated motion of valence electrons and hydrogens in a photoexcited ammonia molecule. The methodology employed in this Letter, which utilizes the charge-pair distribution function from ultrafast electron scattering to retrieve intertwined electron and nucleus dynamics, may open up new opportunities in the study of quantum dynamics for a wide range of molecules.

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• Chemical reactions
• Electronic structure of atoms & molecules
• Light-matter interaction
• Photodissociation
• Scattering theory
• Ultrafast phenomena