@article{e3cec2ba3a20401ba6dbdfbfe74478dc,
title = "Correlation-Driven Transient Hole Dynamics Resolved in Space and Time in the Isopropanol Molecule",
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. ",
author = "T. Barillot and O. Alexander and B. Cooper and T. Driver and D. Garratt and S. Li and {Al Haddad}, A. and A. Sanchez-Gonzalez and M. Ag{\aa}ker and C. Arrell and M. J. Bearpark and N. Berrah and C. Bostedt and J. Bozek and C. Brahms and Bucksbaum, {P. H.} and A. Clark and G. Doumy and R. Feifel and Frasinski, {L. J.} and S. Jarosch and Johnson, {A. S.} and L. Kjellsson and P. Koloren{\v c} and Y. Kumagai and Larsen, {E. W.} and P. Matia-Hernando and M. Robb and J.-E. Rubensson and M. Ruberti and C. Sathe and Squibb, {R. J.} and A. Tan and Tisch, {J. W. G.} and M. Vacher and Walke, {D. J.} and Wolf, {T. J. A.} and D. Wood and V. Zhaunerchyk and P. Walter and T. Osipov and A. Marinelli and Maxwell, {T. J.} and R. Coffee and Lutman, {A. A.} and V. Averbukh and K. Ueda and Cryan, {J. P.} and Marangos, {J. P.}",
note = "Funding Information: Use of the Linac Coherent Light Source (LCLS), SLAC National Accelerator Laboratory, is supported by the U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences (BES) under contract No. DE-AC02-766 76SF00515. The authors acknowledge the invaluable support of the technical and scientific staff of the LCLS at SLAC National Accelerator Laboratory. J. P. M., T. B., O. A., B. C., T. D., D. G., A. S.-G., L. J. F., V. A., M. Robb, M. Ruberti, M. J. B., M. V., J. W. G. T., D. W., S. J., C. Brahms, E. W. L., A. S. J., P. M.-H., and D. J. W. acknowledge funding from EPSRC through Grants No. EP/I032517/1, No. EP/N018680/1, No. EP/R019509/1, and No. EP/T006943/1, and ERC Advanced Grant No. ASTEX (2012-17). A. A. H., G. D., Y. K., and C. Bostedt acknowledge support from the U.S. DOE, Office of BES, Division of Chemical Sciences, Geosciences, and Biosciences under Contract No. DE-AC02- 06CH11357. T. J. A. W., P. H. B. and J. P. C. were supported by the AMOS program in the Chemical Sciences, Geosciences, and Biosciences Division of BES at the DOE. The AMOS program also supported N. B. under Grant No. DE-SC0012376 (UConn). L. K., J.-E. R., M. A., and C. S. gratefully acknowledge support by the Swedish Research Council (VR) under Grants No. 2014-04518 and No. 2018-04088. R. F. and R. J. S. thank the Swedish Research Council and the Knut and Alice Wallenberg Foundation, Sweden for financial support. P. K. acknowledges financial support by the Czech Science Foundation (Project GAR No. 17-10866S). K. U. acknowledges support via the X-ray Free Electron Laser Utilization Research Project and the X-ray Free Electron Laser Priority Strategy Program of MEXT, the Dynamic Alliance for Open Innovation Bridging Human, Environment and Materials Program, and the IMRAM Program of Tohoku University. A. S.-G. is funded by STFC. Publisher Copyright: {\textcopyright} 2021 authors. Published by the American Physical Society.",
year = "2021",
month = sep,
day = "1",
doi = "10.1103/PhysRevX.11.031048",
language = "English",
volume = "11",
journal = "Physical Review X",
issn = "2160-3308",
publisher = "American Physical Society",
number = "3",
}