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Correlation-Driven Transient Hole Dynamics Resolved in Space and Time in the Isopropanol Molecule

Barillot, T; Alexander, O; Cooper, B; Driver, T; Garratt, D; Li, S; Al Haddad, A; ... Kolorenc, P; + view all (2021) Correlation-Driven Transient Hole Dynamics Resolved in Space and Time in the Isopropanol Molecule. Physical Review X , 11 (3) , Article 031048. 10.1103/PhysRevX.11.031048. Green open access

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Abstract

The possibility of suddenly ionized molecules undergoing extremely fast electron hole (or hole) dynamics prior to significant structural change was first recognized more than 20 years ago and termed charge migration. The accurate probing of ultrafast electron hole dynamics requires measurements that have both sufficient temporal resolution and can detect the localization of a specific hole within the molecule. We report an investigation of the dynamics of inner valence hole states in isopropanol where we use an x-ray pump–x-ray probe experiment, with site and state-specific probing of a transient hole state localized near the oxygen atom in the molecule, together with an ab initio theoretical treatment. We record the signature of transient hole dynamics and make the first tentative observation of dynamics driven by frustrated Auger-Meitner transitions. We verify that the effective hole lifetime is consistent with our theoretical prediction. This state-specific measurement paves the way to widespread application for observations of transient hole dynamics localized in space and time in molecules and thus to charge transfer phenomena that are fundamental in chemical and material physics.

Type: Article
Title: Correlation-Driven Transient Hole Dynamics Resolved in Space and Time in the Isopropanol Molecule
Open access status: An open access version is available from UCL Discovery
DOI: 10.1103/PhysRevX.11.031048
Publisher version: https://doi.org/10.1103/PhysRevX.11.031048
Language: English
Additional information: Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article’s title, journal citation, and DOI.
UCL classification: UCL
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Physics and Astronomy
URI: https://discovery.ucl.ac.uk/id/eprint/10134379
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