Attosecond delays in X-ray molecular ionization

Taran Driver (), Miles Mountney, Jun Wang, Lisa Ortmann, Andre Al-Haddad, Nora Berrah, Christoph Bostedt, Elio G. Champenois, Louis F. DiMauro, Joseph Duris, Douglas Garratt, James M. Glownia, Zhaoheng Guo, Daniel Haxton, Erik Isele, Igor Ivanov, Jiabao Ji, Andrei Kamalov, Siqi Li, Ming-Fu Lin, Jon P. Marangos, Razib Obaid, Jordan T. O’Neal, Philipp Rosenberger, Niranjan H. Shivaram, Anna L. Wang, Peter Walter, Thomas J. A. Wolf, Hans Jakob Wörner, Zhen Zhang, Philip H. Bucksbaum, Matthias F. Kling, Alexandra S. Landsman, Robert R. Lucchese, Agapi Emmanouilidou, Agostino Marinelli () and James P. Cryan ()
Additional contact information
Taran Driver: SLAC National Accelerator Laboratory
Miles Mountney: University College London
Jun Wang: SLAC National Accelerator Laboratory
Lisa Ortmann: The Ohio State University
Andre Al-Haddad: Paul Scherrer Institute
Nora Berrah: University of Connecticut
Christoph Bostedt: Paul Scherrer Institute
Elio G. Champenois: SLAC National Accelerator Laboratory
Louis F. DiMauro: The Ohio State University
Joseph Duris: SLAC National Accelerator Laboratory
Douglas Garratt: Imperial College London
James M. Glownia: SLAC National Accelerator Laboratory
Zhaoheng Guo: SLAC National Accelerator Laboratory
Daniel Haxton: KLA Corporation
Erik Isele: SLAC National Accelerator Laboratory
Igor Ivanov: Institute for Basic Science
Jiabao Ji: ETH Zurich
Andrei Kamalov: SLAC National Accelerator Laboratory
Siqi Li: SLAC National Accelerator Laboratory
Ming-Fu Lin: SLAC National Accelerator Laboratory
Jon P. Marangos: Imperial College London
Razib Obaid: University of Connecticut
Jordan T. O’Neal: SLAC National Accelerator Laboratory
Philipp Rosenberger: Ludwig-Maximilians-Universität
Niranjan H. Shivaram: SLAC National Accelerator Laboratory
Anna L. Wang: SLAC National Accelerator Laboratory
Peter Walter: SLAC National Accelerator Laboratory
Thomas J. A. Wolf: SLAC National Accelerator Laboratory
Hans Jakob Wörner: ETH Zurich
Zhen Zhang: SLAC National Accelerator Laboratory
Philip H. Bucksbaum: SLAC National Accelerator Laboratory
Matthias F. Kling: SLAC National Accelerator Laboratory
Alexandra S. Landsman: The Ohio State University
Robert R. Lucchese: Purdue University
Agapi Emmanouilidou: University College London
Agostino Marinelli: SLAC National Accelerator Laboratory
James P. Cryan: SLAC National Accelerator Laboratory

Nature, 2024, vol. 632, issue 8026, 762-767

Abstract: 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 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.

Date: 2024
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DOI: 10.1038/s41586-024-07771-9

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