Attosecond spectroscopy of size-resolved water clusters

Gong, Xiaochun; Heck, Saijoscha; Jelovina, Denis; Perry, Conaill; Zinchenko, Kristina; Lucchese, Robert; Wörner, Hans Jakob

doi:10.1038/s41586-022-05039-8

Attosecond spectroscopy of size-resolved water clusters

Journal Article · Tue Jul 12 00:00:00 EDT 2022 · Nature (London)

DOI:https://doi.org/10.1038/s41586-022-05039-8· OSTI ID:1974750

^[1]; ^[2]; Jelovina, Denis ^[2]; ^[2]; Zinchenko, Kristina ^[2]; ^[3]; ^[2]

Eidgenoessische Technische Hochschule (ETH), Zurich (Switzerland); East China Normal Univ. (ECNU), Shanghai (China)
Eidgenoessische Technische Hochschule (ETH), Zurich (Switzerland)
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Chemical Sciences Division

Electron dynamics in water are of fundamental importance for a broad range of phenomena, but their real-time study faces numerous conceptual and methodological challenges. Here, in this paper, 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 delays 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.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1974750

Journal Information:: Nature (London), Journal Name: Nature (London) Journal Issue: 7927 Vol. 609; ISSN 0028-0836

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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