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

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...

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Autores principales: T. Barillot, O. Alexander, B. Cooper, T. Driver, D. Garratt, S. Li, A. Al Haddad, A. Sanchez-Gonzalez, M. Agåker, C. Arrell, M. J. Bearpark, N. Berrah, C. Bostedt, J. Bozek, C. Brahms, P. H. Bucksbaum, A. Clark, G. Doumy, R. Feifel, L. J. Frasinski, S. Jarosch, A. S. Johnson, L. Kjellsson, P. Kolorenč, Y. Kumagai, E. W. Larsen, P. Matia-Hernando, M. Robb, J.-E. Rubensson, M. Ruberti, C. Sathe, R. J. Squibb, A. Tan, J. W. G. Tisch, M. Vacher, D. J. Walke, T. J. A. Wolf, D. Wood, V. Zhaunerchyk, P. Walter, T. Osipov, A. Marinelli, T. J. Maxwell, R. Coffee, A. A. Lutman, V. Averbukh, K. Ueda, J. P. Cryan, J. P. Marangos
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Publicado: American Physical Society 2021
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spelling oai:doaj.org-article:9125dfe7b71b4902b383d1eaa3c5b4f52021-12-02T16:35:51ZCorrelation-Driven Transient Hole Dynamics Resolved in Space and Time in the Isopropanol Molecule10.1103/PhysRevX.11.0310482160-3308https://doaj.org/article/9125dfe7b71b4902b383d1eaa3c5b4f52021-09-01T00:00:00Zhttp://doi.org/10.1103/PhysRevX.11.031048http://doi.org/10.1103/PhysRevX.11.031048https://doaj.org/toc/2160-3308The 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.T. BarillotO. AlexanderB. CooperT. DriverD. GarrattS. LiA. Al HaddadA. Sanchez-GonzalezM. AgåkerC. ArrellM. J. BearparkN. BerrahC. BostedtJ. BozekC. BrahmsP. H. BucksbaumA. ClarkG. DoumyR. FeifelL. J. FrasinskiS. JaroschA. S. JohnsonL. KjellssonP. KolorenčY. KumagaiE. W. LarsenP. Matia-HernandoM. RobbJ.-E. RubenssonM. RubertiC. SatheR. J. SquibbA. TanJ. W. G. TischM. VacherD. J. WalkeT. J. A. WolfD. WoodV. ZhaunerchykP. WalterT. OsipovA. MarinelliT. J. MaxwellR. CoffeeA. A. LutmanV. AverbukhK. UedaJ. P. CryanJ. P. MarangosAmerican Physical SocietyarticlePhysicsQC1-999ENPhysical Review X, Vol 11, Iss 3, p 031048 (2021)
institution DOAJ
collection DOAJ
language EN
topic Physics
QC1-999
spellingShingle Physics
QC1-999
T. Barillot
O. Alexander
B. Cooper
T. Driver
D. Garratt
S. Li
A. Al Haddad
A. Sanchez-Gonzalez
M. Agåker
C. Arrell
M. J. Bearpark
N. Berrah
C. Bostedt
J. Bozek
C. Brahms
P. H. Bucksbaum
A. Clark
G. Doumy
R. Feifel
L. J. Frasinski
S. Jarosch
A. S. Johnson
L. Kjellsson
P. Kolorenč
Y. Kumagai
E. W. Larsen
P. Matia-Hernando
M. Robb
J.-E. Rubensson
M. Ruberti
C. Sathe
R. J. Squibb
A. Tan
J. W. G. Tisch
M. Vacher
D. J. Walke
T. J. A. Wolf
D. Wood
V. Zhaunerchyk
P. Walter
T. Osipov
A. Marinelli
T. J. Maxwell
R. Coffee
A. A. Lutman
V. Averbukh
K. Ueda
J. P. Cryan
J. P. Marangos
Correlation-Driven Transient Hole Dynamics Resolved in Space and Time in the Isopropanol Molecule
description 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.
format article
author T. Barillot
O. Alexander
B. Cooper
T. Driver
D. Garratt
S. Li
A. Al Haddad
A. Sanchez-Gonzalez
M. Agåker
C. Arrell
M. J. Bearpark
N. Berrah
C. Bostedt
J. Bozek
C. Brahms
P. H. Bucksbaum
A. Clark
G. Doumy
R. Feifel
L. J. Frasinski
S. Jarosch
A. S. Johnson
L. Kjellsson
P. Kolorenč
Y. Kumagai
E. W. Larsen
P. Matia-Hernando
M. Robb
J.-E. Rubensson
M. Ruberti
C. Sathe
R. J. Squibb
A. Tan
J. W. G. Tisch
M. Vacher
D. J. Walke
T. J. A. Wolf
D. Wood
V. Zhaunerchyk
P. Walter
T. Osipov
A. Marinelli
T. J. Maxwell
R. Coffee
A. A. Lutman
V. Averbukh
K. Ueda
J. P. Cryan
J. P. Marangos
author_facet T. Barillot
O. Alexander
B. Cooper
T. Driver
D. Garratt
S. Li
A. Al Haddad
A. Sanchez-Gonzalez
M. Agåker
C. Arrell
M. J. Bearpark
N. Berrah
C. Bostedt
J. Bozek
C. Brahms
P. H. Bucksbaum
A. Clark
G. Doumy
R. Feifel
L. J. Frasinski
S. Jarosch
A. S. Johnson
L. Kjellsson
P. Kolorenč
Y. Kumagai
E. W. Larsen
P. Matia-Hernando
M. Robb
J.-E. Rubensson
M. Ruberti
C. Sathe
R. J. Squibb
A. Tan
J. W. G. Tisch
M. Vacher
D. J. Walke
T. J. A. Wolf
D. Wood
V. Zhaunerchyk
P. Walter
T. Osipov
A. Marinelli
T. J. Maxwell
R. Coffee
A. A. Lutman
V. Averbukh
K. Ueda
J. P. Cryan
J. P. Marangos
author_sort T. Barillot
title Correlation-Driven Transient Hole Dynamics Resolved in Space and Time in the Isopropanol Molecule
title_short Correlation-Driven Transient Hole Dynamics Resolved in Space and Time in the Isopropanol Molecule
title_full Correlation-Driven Transient Hole Dynamics Resolved in Space and Time in the Isopropanol Molecule
title_fullStr Correlation-Driven Transient Hole Dynamics Resolved in Space and Time in the Isopropanol Molecule
title_full_unstemmed Correlation-Driven Transient Hole Dynamics Resolved in Space and Time in the Isopropanol Molecule
title_sort correlation-driven transient hole dynamics resolved in space and time in the isopropanol molecule
publisher American Physical Society
publishDate 2021
url https://doaj.org/article/9125dfe7b71b4902b383d1eaa3c5b4f5
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