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Simultaneous observation of nuclear and electronic dynamics by ultrafast electron diffraction
Ist Teil von
Science (American Association for the Advancement of Science), 2020-05, Vol.368 (6493), p.885-889
Ort / Verlag
United States: The American Association for the Advancement of Science
Erscheinungsjahr
2020
Quelle
American Association for the Advancement of Science
Beschreibungen/Notizen
Simultaneous observation of nuclear and electronic motion is crucial for a complete understanding of molecular dynamics in excited electronic states. It is challenging for a single experiment to independently follow both electronic and nuclear dynamics at the same time. Here we show that ultrafast electron diffraction can be used to simultaneously record both electronic and nuclear dynamics in isolated pyridine molecules, naturally disentangling the two components. Electronic state changes (S
→S
internal conversion) were reflected by a strong transient signal in small-angle inelastic scattering, and nuclear structural changes (ring puckering) were monitored by large-angle elastic diffraction. Supported by ab initio nonadiabatic molecular dynamics and diffraction simulations, our experiment provides a clear view of the interplay between electronic and nuclear dynamics of the photoexcited pyridine molecule.