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Shake-Down Spectroscopy as State- and Site-Specific Probe of Ultrafast Chemical Dynamics.


ABSTRACT: Tracking the multifarious ultrafast electronic and structural changes occurring in a molecule during a photochemical transformation is a challenging endeavor that benefits from recent experimental and computational progress in time-resolved techniques. Measurements of valence electronic states, which provide a global picture of the bonding structure of the molecule, and core electronic states, which provide insight into the local environment, traditionally require different approaches and are often studied separately. Here, we demonstrate that X-ray pulses from a seeded free-electron laser (FEL) enable the measurement of high-resolution, time-resolved X-ray photoelectron spectra (XPS) that capture weak satellite states resulting from shake-down processes in a valence-excited molecule. This

SUBMITTER: Thompson HJ 

PROVIDER: S-EPMC12426938 | biostudies-literature | 2025 Sep

REPOSITORIES: biostudies-literature