Attosecond delays in X-ray molecular ionization

Taran Driver^{1

2}, Miles Mountney³, Jun Wang^{4

5

6}, Lisa Ortmann⁷, Andre Al-Haddad⁸, Nora Berrah⁹, Christoph Bostedt^{8

10}, Elio G Champenois⁴, Louis F DiMauro⁷, Joseph Duris⁵, Douglas Garratt¹¹, James M Glownia⁵, Zhaoheng Guo^{5

6}, Daniel Haxton¹², Erik Isele^{4

5

6}, Igor Ivanov¹³, Jiabao Ji¹⁴, Andrei Kamalov⁴, Siqi Li⁵, Ming-Fu Lin⁵, Jon P Marangos¹¹, Razib Obaid⁹, Jordan T O'Neal⁴, Philipp Rosenberger^{15

16}, Niranjan H Shivaram^{5

17

18}, Anna L Wang⁴, Peter Walter⁵, Thomas J A Wolf^{4

5}, Hans Jakob Wörner¹⁴, Zhen Zhang⁵, Philip H Bucksbaum^{4

6}, Matthias F Kling^{4

5

15

16}, Alexandra S Landsman⁷, Robert R Lucchese^{18

19}, Agapi Emmanouilidou³, Agostino Marinelli^{20

21}, James P Cryan^{22

23}

Affiliations

¹ Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, CA, USA. tdriver@stanford.edu.
² Linac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, CA, USA. tdriver@stanford.edu.
³ Department of Physics and Astronomy, University College London, London, UK.
⁴ Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, CA, USA.
⁵ Linac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, CA, USA.
⁶ Department of Applied Physics, Stanford University, Stanford, CA, USA.
⁷ Department of Physics, The Ohio State University, Columbus, OH, USA.
⁸ Paul Scherrer Institute, Villigen, Switzerland.
⁹ Department of Physics, University of Connecticut, Storrs, CT, USA.
¹⁰ LUXS Laboratory for Ultrafast X-ray Sciences, Institute of Chemical Sciences and Engineering, École Polytechnique Fédérale de Lausanne (EPFL), Lausanne, Switzerland.
¹¹ The Blackett Laboratory, Imperial College London, London, UK.
¹² KLA Corporation, Milpitas, CA, USA.
¹³ Center for Relativistic Laser Science, Institute for Basic Science, Gwangju, Korea.
¹⁴ Laboratorium für Physikalische Chemie, ETH Zurich, Zurich, Switzerland.
¹⁵ Physics Department, Ludwig-Maximilians-Universität, Munich, Germany.
¹⁶ Max Planck Institute of Quantum Optics, Garching, Germany.
¹⁷ Department of Physics and Astronomy, Purdue University, West Lafayette, IN, USA.
¹⁸ Purdue Quantum Science and Engineering Institute, Purdue University, West Lafayette, IN, USA.
¹⁹ Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA, USA.
²⁰ Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, CA, USA. marinelli@slac.stanford.edu.
²¹ Linac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, CA, USA. marinelli@slac.stanford.edu.
²² Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, CA, USA. jcryan@slac.stanford.edu.
²³ Linac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, CA, USA. jcryan@slac.stanford.edu.

PMID: 39169246
DOI: 10.1038/s41586-024-07771-9

Free article

Attosecond delays in X-ray molecular ionization

Taran Driver et al. Nature. 2024 Aug.

Free article

. 2024 Aug;632(8026):762-767.

doi: 10.1038/s41586-024-07771-9. Epub 2024 Aug 21.

Authors

Affiliations

¹ Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, CA, USA. tdriver@stanford.edu.
² Linac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, CA, USA. tdriver@stanford.edu.
³ Department of Physics and Astronomy, University College London, London, UK.
⁴ Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, CA, USA.
⁵ Linac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, CA, USA.
⁶ Department of Applied Physics, Stanford University, Stanford, CA, USA.
⁷ Department of Physics, The Ohio State University, Columbus, OH, USA.
⁸ Paul Scherrer Institute, Villigen, Switzerland.
⁹ Department of Physics, University of Connecticut, Storrs, CT, USA.
¹⁰ LUXS Laboratory for Ultrafast X-ray Sciences, Institute of Chemical Sciences and Engineering, École Polytechnique Fédérale de Lausanne (EPFL), Lausanne, Switzerland.
¹¹ The Blackett Laboratory, Imperial College London, London, UK.
¹² KLA Corporation, Milpitas, CA, USA.
¹³ Center for Relativistic Laser Science, Institute for Basic Science, Gwangju, Korea.
¹⁴ Laboratorium für Physikalische Chemie, ETH Zurich, Zurich, Switzerland.
¹⁵ Physics Department, Ludwig-Maximilians-Universität, Munich, Germany.
¹⁶ Max Planck Institute of Quantum Optics, Garching, Germany.
¹⁷ Department of Physics and Astronomy, Purdue University, West Lafayette, IN, USA.
¹⁸ Purdue Quantum Science and Engineering Institute, Purdue University, West Lafayette, IN, USA.
¹⁹ Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA, USA.
²⁰ Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, CA, USA. marinelli@slac.stanford.edu.
²¹ Linac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, CA, USA. marinelli@slac.stanford.edu.
²² Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, CA, USA. jcryan@slac.stanford.edu.
²³ Linac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, CA, USA. jcryan@slac.stanford.edu.

PMID: 39169246
DOI: 10.1038/s41586-024-07771-9

Abstract

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.

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References

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1. Huppert, M., Jordan, I., Baykusheva, D., Conta, A. & Wörner, H. J. Attosecond delays in molecular photoionization. Phys. Rev. Lett. 117, 093001 (2016). - PubMed - DOI
1. Vos, J. et al. Orientation-dependent stereo Wigner time delay and electron localization in a small molecule. Science 360, 1326–1330 (2018). - PubMed - DOI
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1. Kamalov, A., Wang, A. L., Bucksbaum, P. H., Haxton, D. J. & Cryan, J. P. Electron correlation effects in attosecond photoionization of CO₂. Phys. Rev. A 102, 023118 (2020). - DOI

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Attosecond delays in X-ray molecular ionization

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Attosecond delays in X-ray molecular ionization

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Abstract

References

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