Attosecond Photoionization Dynamics: from Molecules over Clusters to the Liquid Phase

Authors

  • Xiaochun Gong State Key laboratory of precision spectroscopy, East China Normal University, 500 Dongchuan Road, Shanghai, China
  • Inga Jordan Laboratorium für Physikalische Chemie, ETH Zürich, CH-8093 Zürich
  • Martin Huppert Paul Scherrer Institute, Forschungsstrasse 111, 5232 Villigen PSI
  • Saijoscha Heck Laboratorium für Physikalische Chemie, ETH Zürich, CH-8093 Zürich
  • Denitsa Baykusheva Department of Physics, Harvard University 17, Oxford Street, Cambridge, MA 02138
  • Denis Jelovina Laboratorium für Physikalische Chemie, ETH Zürich, CH-8093 Zürich
  • Axel Schild Laboratorium für Physikalische Chemie, ETH Zürich, CH-8093 Zürich https://orcid.org/0000-0002-0852-0938
  • Hans Jakob Wörner Laboratorium für Physikalische Chemie, ETH Zürich, CH-8093 Zürich

DOI:

https://doi.org/10.2533/chimia.2022.520

PMID:

38069721

Keywords:

attosecond spectroscopy, photoionization delays, molecular photoionization, water clusters, liquid water, electron scattering

Abstract

Photoionization is a process taking place on attosecond time scales. How its properties evolve from isolated particles to the condensed phase is an open question of both fundamental and practical relevance. Here, we review recent work that has advanced the study of photoionization dynamics from atoms to molecules, clusters and the liquid phase. The first measurements of molecular photoionization delays have revealed the attosecond dynamics of electron emission from a molecular shape resonance and their sensitivity to the molecular potential. Using electron-ion coincidence spectroscopy these measurements have been extended from isolated molecules to clusters. A continuous increase of the delays with the water-cluster size has been observed up to a size of 4-5 molecules, followed by a saturation towards larger clusters. Comparison with calculations has revealed a correlation of the time delay with the spatial extension of the created electron hole. Using cylindrical liquid-microjet techniques, these measurements have also been extended to liquid water, revealing a delay relative to isolated water molecules that was very similar to the largest water clusters studied. Detailed modeling based on Monte-Carlo simulations confirmed that these delays are dominated by the contributions of the first two solvation shells, which agrees with the results of the cluster measurements. These combined results open the perspective of experimentally characterizing the delocalization of electronic wave functions in complex systems and studying their evolution on attosecond time scales.

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Published

2022-06-29

How to Cite

[1]
X. Gong, I. Jordan, M. Huppert, S. Heck, D. Baykusheva, D. Jelovina, A. Schild, H. J. Wörner, Chimia 2022, 76, 520, DOI: 10.2533/chimia.2022.520.