Correlation-driven transient hole dynamics resolved in space and time in the isopropanol molecule
File(s)PhysRevX.11.031048.pdf (1.34 MB)
Published version
Author(s)
Type
Journal Article
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.
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.
Date Issued
2021-09-01
Date Acceptance
2021-06-21
Citation
Physical Review X, 2021, 11, pp.1-15
ISSN
2160-3308
Publisher
American Physical Society
Start Page
1
End Page
15
Journal / Book Title
Physical Review X
Volume
11
Copyright Statement
© The Author(s).
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.
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.
Sponsor
Engineering & Physical Science Research Council (EPSRC)
Commission of the European Communities
Engineering and Physical Sciences Research Council
Engineering & Physical Science Research Council (EPSRC)
Identifier
https://journals.aps.org/prx/abstract/10.1103/PhysRevX.11.031048
Grant Number
EP/I032517/1
290467
EP/R019509/1
EP/T006943/1
Subjects
Science & Technology
Physical Sciences
Physics, Multidisciplinary
Physics
SURFACE-HOPPING PROGRAM
CHARGE MIGRATION
NEWTON-X
ATTOSECOND
SPECTROSCOPY
FEMTOSECOND
IONIZATION
physics.chem-ph
physics.chem-ph
quant-ph
0201 Astronomical and Space Sciences
0204 Condensed Matter Physics
0206 Quantum Physics
Publication Status
Published
Date Publish Online
2021-09-01