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

Barillot, T. R. ; Alexander, O. ; Cooper, B. ; Driver, T. ; Garratt, D. ; Li, S. ; Al Haddad, A. ; Sanchez-Gonzalez, A. ; Agåker, M. LU and Arrell, C. , et al. (2021) In Physical Review X 11(3).
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... (More)

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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organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Physical Review X
volume
11
issue
3
article number
031048
publisher
American Physical Society
external identifiers
  • scopus:85114415386
ISSN
2160-3308
DOI
10.1103/PhysRevX.11.031048
language
English
LU publication?
yes
id
c91298de-d6c6-42a6-bd5d-5e0af878edfb
date added to LUP
2021-10-05 14:52:53
date last changed
2022-04-27 04:26:46
@article{c91298de-d6c6-42a6-bd5d-5e0af878edfb,
  abstract     = {{<p>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. </p>}},
  author       = {{Barillot, T. R. and Alexander, O. and Cooper, B. and Driver, T. and Garratt, D. and Li, S. and Al Haddad, A. and Sanchez-Gonzalez, A. and Agåker, M. and Arrell, C. and Bearpark, M. J. and Berrah, N. and Bostedt, C. and Bozek, J. and Brahms, C. and Bucksbaum, P. H. and Clark, A. and Doumy, G. and Feifel, R. and Frasinski, L. J. and Jarosch, S. and Johnson, A. S. and Kjellsson, L. and Kolorenč, P. and Kumagai, Y. and Larsen, E. W. and Matia-Hernando, P. and Robb, M. and Rubensson, J. E. and Ruberti, M. and Sathe, C. and Squibb, R. J. and Tan, A. and Tisch, J. W.G. and Vacher, M. and Walke, D. J. and Wolf, T. J.A. and Wood, D. and Zhaunerchyk, V. and Walter, P. and Osipov, T. and Marinelli, A. and Maxwell, T. J. and Coffee, R. and Lutman, A. A. and Averbukh, V. and Ueda, K. and Cryan, J. P. and Marangos, J. P.}},
  issn         = {{2160-3308}},
  language     = {{eng}},
  month        = {{09}},
  number       = {{3}},
  publisher    = {{American Physical Society}},
  series       = {{Physical Review X}},
  title        = {{Correlation-Driven Transient Hole Dynamics Resolved in Space and Time in the Isopropanol Molecule}},
  url          = {{http://dx.doi.org/10.1103/PhysRevX.11.031048}},
  doi          = {{10.1103/PhysRevX.11.031048}},
  volume       = {{11}},
  year         = {{2021}},
}