Probing Valence Electron and Hydrogen Dynamics Using Charge-Pair Imaging with Ultrafast Electron Diffraction

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 (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.