Correlation-Driven Transient Hole Dynamics Resolved in Space and Time in the Isopropanol Molecule
| Autor: | Siqi Li, Ludvig Kjellsson, A. Clark, Leszek J. Frasinski, Morgane Vacher, Agostino Marinelli, Alberto Lutman, Richard J. Squibb, Douglas Garratt, Sebastian Jarosch, Raimund Feifel, Michael J. Bearpark, Esben Witting Larsen, James P. Cryan, Ryan Coffee, J. P. Marangos, Oliver Alexander, Michael A. Robb, M. Ruberti, Marcus Agåker, Kiyoshi Ueda, Taran Driver, John D. Bozek, Christopher Arrell, Alvaro Sanchez-Gonzalez, Christoph Bostedt, T. J. Maxwell, Yoshiaki Kumagai, Vitali Zhaunerchyk, Timur Osipov, A. Tan, Philip H. Bucksbaum, D. J. Walke, B. D. Cooper, Andre Al Haddad, Thomas J. A. Wolf, Paloma Matia-Hernando, Jan-Erik Rubensson, Christian Brahms, Darien Wood, T. Barillot, Přemysl Kolorenč, Nora Berrah, Allan S. Johnson, Peter Walter, Conny Såthe, Vitali Averbukh, Gilles Doumy, John W. G. Tisch |
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| Přispěvatelé: | Chimie Et Interdisciplinarité : Synthèse, Analyse, Modélisation (CEISAM), Université de Nantes - UFR des Sciences et des Techniques (UN UFR ST), Université de Nantes (UN)-Université de Nantes (UN)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), Engineering & Physical Science Research Council (EPSRC), Commission of the European Communities, Engineering and Physical Sciences Research Council |
| Jazyk: | angličtina |
| Rok vydání: | 2021 |
| Předmět: |
spectroscopy
attosecond Attosecond QC1-999 Astrophysics::High Energy Astrophysical Phenomena Physics Multidisciplinary physics.chem-ph 0204 Condensed Matter Physics Ab initio General Physics and Astronomy FOS: Physical sciences newton-x 02 engineering and technology Electron hole 01 natural sciences Molecular physics quant-ph Ionization Physics - Chemical Physics 0201 Astronomical and Space Sciences 0103 physical sciences ionization Molecule 010306 general physics 0206 Quantum Physics femtosecond ComputingMilieux_MISCELLANEOUS Physics Chemical Physics (physics.chem-ph) Quantum Physics Science & Technology Valence (chemistry) 021001 nanoscience & nanotechnology Condensed Matter Physics surface-hopping program Temporal resolution Physical Sciences charge migration Transient (oscillation) [PHYS.PHYS.PHYS-CHEM-PH]Physics [physics]/Physics [physics]/Chemical Physics [physics.chem-ph] 0210 nano-technology Quantum Physics (quant-ph) Den kondenserade materiens fysik |
| Zdroj: | Physical Review X, Vol 11, Iss 3, p 031048 (2021) Physical Review X Physical Review X, American Physical Society, 2021, 11 (3), ⟨10.1103/PhysRevX.11.031048⟩ |
| ISSN: | 2160-3308 |
| DOI: | 10.1103/PhysRevX.11.031048⟩ |
| Popis: | 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. (Less) |
| Databáze: | OpenAIRE |
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