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  4. Correlation-Driven Transient Hole Dynamics Resolved in Space and Time in the Isopropanol Molecule
 
research article

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

Barillot, T.
•
Alexander, O.
•
Cooper, B.
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September 1, 2021
Physical Review X

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.

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Type
research article
DOI
10.1103/PhysRevX.11.031048
Web of Science ID

WOS:000692103200001

Author(s)
Barillot, T.
Alexander, O.
Cooper, B.
Driver, T.
Garratt, D.
Li, S.
Al Haddad, A.
Sanchez-Gonzalez, A.
Agaker, M.
Arrell, C.
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Date Issued

2021-09-01

Published in
Physical Review X
Volume

11

Issue

3

Article Number

031048

Subjects

Physics, Multidisciplinary

•

Physics

•

surface-hopping program

•

charge migration

•

newton-x

•

attosecond

•

spectroscopy

•

femtosecond

•

ionization

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

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Available on Infoscience
September 11, 2021
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/181384
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