The photoelectric effect is not truly instantaneous but exhibits attosecond delays that can reveal complex molecular dynamics(1-7). Sub-femtosecond-duration light pulses provide the requisite tools to resolve the dynamics of photoionization(8-12). Accordingly, the past decade has produced a large volume of work on photoionization delays following single-photon absorption of an extreme ultraviolet photon. However, the measurement of time-resolved core-level photoionization remained out of reach. The required X-ray photon energies needed for core-level photoionization were not available with attosecond tabletop sources. Here we report measurements of the X-ray photoemission delay of core-level electrons, with unexpectedly large delays, ranging up to 700 as in NO near the oxygen K-shell threshold. These measurements exploit attosecond soft X-ray pulses from a free-electron laser to scan across the entire region near the K-shell threshold. Furthermore, we find that the delay spectrum is richly modulated, suggesting several contributions, including transient trapping of the photoelectron owing to shape resonances, collisions with the Auger-Meitner electron that is emitted in the rapid non-radiative relaxation of the molecule and multi-electron scattering effects. The results demonstrate how X-ray attosecond experiments, supported by comprehensive theoretical modelling, can unravel the complex correlated dynamics of core-level photoionization.
WOS:001300596600010
39169246
Stanford University
University of London
Stanford University
University System of Ohio
Swiss Federal Institutes of Technology Domain
University of Connecticut
École Polytechnique Fédérale de Lausanne
Stanford University
University System of Ohio
Stanford University
2024-08-22
632
8026
REVIEWED
EPFL
| Funder | Funding(s) | Grant Number | Grant URL |
United States Department of Energy (DOE) | DE-AC02-76SF00515 | ||
United States Department of Energy (DOE) | |||
Accelerator and Detector Research Program of the Department of Energy, Basic Energy Sciences division | |||
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