Attosecond delays in X-ray molecular ionization.
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abstract
The photoelectric effect is not truly instantaneous but exhibits attosecond delays that can reveal complex molecular dynamics1-7. Sub-femtosecond-duration light pulses provide the requisite tools to resolve the dynamics of photoionization8-12. 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 700as 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.
Driver, T., Mountney, M., Wang, J., Ortmann, L., Al-Haddad, A., Berrah, N., ... Cryan, J. P.
complete list of authors
Driver, Taran||Mountney, Miles||Wang, Jun||Ortmann, Lisa||Al-Haddad, Andre||Berrah, Nora||Bostedt, Christoph||Champenois, Elio G||DiMauro, Louis F||Duris, Joseph||Garratt, Douglas||Glownia, James M||Guo, Zhaoheng||Haxton, Daniel||Isele, Erik||Ivanov, Igor||Ji, Jiabao||Kamalov, Andrei||Li, Siqi||Lin, Ming-Fu||Marangos, Jon P||Obaid, Razib||O'Neal, Jordan T||Rosenberger, Philipp||Shivaram, Niranjan H||Wang, Anna L||Walter, Peter||Wolf, Thomas JA||Wörner, Hans Jakob||Zhang, Zhen||Bucksbaum, Philip H||Kling, Matthias F||Landsman, Alexandra S||Lucchese, Robert R||Emmanouilidou, Agapi||Marinelli, Agostino||Cryan, James P
