Attosecond spectroscopy of size-resolved water clusters

Xiaochun Gong, Saijoscha Heck, Denis Jelovina, Conaill Perry, Kristina Zinchenko, Robert Lucchese and Hans Jakob Wörner ()
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Xiaochun Gong: ETH Zürich
Saijoscha Heck: ETH Zürich
Denis Jelovina: ETH Zürich
Conaill Perry: ETH Zürich
Kristina Zinchenko: ETH Zürich
Robert Lucchese: Lawrence Berkeley National Laboratory
Hans Jakob Wörner: ETH Zürich

Nature, 2022, vol. 609, issue 7927, 507-511

Abstract: Abstract Electron dynamics in water are of fundamental importance for a broad range of phenomena1–3, but their real-time study faces numerous conceptual and methodological challenges4–6. Here we introduce attosecond size-resolved cluster spectroscopy and build up a molecular-level understanding of the attosecond electron dynamics in water. We measure the effect that the addition of single water molecules has on the photoionization time delays7–9 of water clusters. We find a continuous increase of the delay for clusters containing up to four to five molecules and little change towards larger clusters. We show that these delays are proportional to the spatial extension of the created electron hole, which first increases with cluster size and then partially localizes through the onset of structural disorder that is characteristic of large clusters and bulk liquid water. These results indicate a previously unknown sensitivity of photoionization delays to electron-hole delocalization and indicate a direct link between electronic structure and attosecond photoionization dynamics. Our results offer new perspectives for studying electron-hole delocalization and its attosecond dynamics.

Date: 2022
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DOI: 10.1038/s41586-022-05039-8

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