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

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, Thomas 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
September 2021
Cite DOI URL

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.

Type
Journal article
Publication
Physical Review X
Thomas Wolf
Thomas Wolf
Staff Scientist

My research is focused on discovering structure-function relationships in ultrafast photochemistry to better understand and eventually control this type of reactions.