Attosecond delays in X-ray molecular ionization

• 成果类型: Article
• 署名作者: 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 J. A.; Woerner, Hans Jakob; Zhang, Zhen; Bucksbaum, Philip H.; Kling, Matthias F.; Landsman, Alexandra S.; Lucchese, Robert R.; Emmanouilidou, Agapi; Marinelli, Agostino; Cryan, James P.
• 署名单位: Stanford University; United States Department of Energy (DOE); SLAC National Accelerator Laboratory; Stanford University; United States Department of Energy (DOE); SLAC National Accelerator Laboratory; University of London; University College London; Stanford University; University System of Ohio; Ohio State University; Swiss Federal Institutes of Technology Domain; Paul Scherrer Institute; University of Connecticut; Swiss Federal Institutes of Technology Domain; Ecole Polytechnique Federale de Lausanne; Imperial College London; KLA Corporation; Institute for Basic Science - Korea (IBS); Swiss Federal Institutes of Technology Domain; ETH Zurich; University of Munich; Max Planck Society; Purdue University System; Purdue University; Purdue University System; Purdue University; United States Department of Energy (DOE); Lawrence Berkeley National Laboratory
• 刊物名称: Nature
• ISSN/ISSBN: 0028-4584
• DOI: 10.1038/s41586-024-07771-9
• 发表日期: 2024-08-22
• 关键词: time; photoionization; atoms

摘要

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.