title: Imaging charge transfer in iodomethane upon x-ray photoabsorption.
abstract: Studies of charge transfer are often hampered by difficulties in determining the charge localization at a given time. Here, we used ultrashort x-ray free-electron laser pulses to image charge rearrangement dynamics within gas-phase iodomethane molecules during dissociation induced by a synchronized near-infrared (NIR) laser pulse. Inner-shell photoionization creates positive charge, which is initially localized on the iodine atom. We map the electron transfer between the methyl and iodine fragments as a function of their interatomic separation set by the NIR-x-ray delay. We observe signatures of electron transfer for distances up to 20 angstroms and show that a realistic estimate of its effective spatial range can be obtained from a classical over-the-barrier model. The presented technique is applicable for spatiotemporal imaging of charge transfer dynamics in a wide range of molecular systems.
authors.affiliation: Deutsches Elektronen-Synchrotron (DESY), 22607 Hamburg, Germany. Max Planck Advanced Study Group at CFEL, 22607 Hamburg, Germany. Max-Planck-Institut für Kernphysik, 69117 Heidelberg, Germany. benjamin.erk@desy.de rudenko@phys.ksu.edu.
authors.forename: Benjamin
authors.initials: B
authors.lastname: Erk
authors.affiliation: Deutsches Elektronen-Synchrotron (DESY), 22607 Hamburg, Germany. Max Planck Advanced Study Group at CFEL, 22607 Hamburg, Germany. Max-Planck-Institut für Kernphysik, 69117 Heidelberg, Germany.
authors.forename: Rebecca
authors.initials: R
authors.lastname: Boll
authors.affiliation: Center for Free-Electron Laser Science (CFEL), DESY, 22607 Hamburg, Germany.
authors.forename: Sebastian
authors.initials: S
authors.lastname: Trippel
authors.affiliation: Deutsches Elektronen-Synchrotron (DESY), 22607 Hamburg, Germany. Max Planck Advanced Study Group at CFEL, 22607 Hamburg, Germany. Max-Planck-Institut für Kernphysik, 69117 Heidelberg, Germany.
authors.forename: Denis
authors.initials: D
authors.lastname: Anielski
authors.affiliation: Max Planck Advanced Study Group at CFEL, 22607 Hamburg, Germany. Max-Planck-Institut für Medizinische Forschung, 69120 Heidelberg, Germany.
authors.forename: Lutz
authors.initials: L
authors.lastname: Foucar
authors.affiliation: Max Planck Advanced Study Group at CFEL, 22607 Hamburg, Germany. Max-Planck-Institut für Kernphysik, 69117 Heidelberg, Germany. Physikalisch-Technische Bundesanstalt, 38116 Braunschweig, Germany.
authors.forename: Benedikt
authors.initials: B
authors.lastname: Rudek
authors.affiliation: Max Planck Advanced Study Group at CFEL, 22607 Hamburg, Germany. Max-Planck-Institut für Kernphysik, 69117 Heidelberg, Germany.
authors.forename: Sascha W
authors.initials: SW
authors.lastname: Epp
authors.affiliation: Linac Coherent Light Source, SLAC National Accelerator Laboratory, 94025 Menlo Park, CA, USA.
authors.forename: Ryan
authors.initials: R
authors.lastname: Coffee
authors.affiliation: Linac Coherent Light Source, SLAC National Accelerator Laboratory, 94025 Menlo Park, CA, USA.
authors.forename: Sebastian
authors.initials: S
authors.lastname: Carron
authors.affiliation: Linac Coherent Light Source, SLAC National Accelerator Laboratory, 94025 Menlo Park, CA, USA.
authors.forename: Sebastian
authors.initials: S
authors.lastname: Schorb
authors.affiliation: Linac Coherent Light Source, SLAC National Accelerator Laboratory, 94025 Menlo Park, CA, USA.
authors.forename: Ken R
authors.initials: KR
authors.lastname: Ferguson
authors.affiliation: Linac Coherent Light Source, SLAC National Accelerator Laboratory, 94025 Menlo Park, CA, USA.
authors.forename: Michele
authors.initials: M
authors.lastname: Swiggers
authors.affiliation: Linac Coherent Light Source, SLAC National Accelerator Laboratory, 94025 Menlo Park, CA, USA.
authors.forename: John D
authors.initials: JD
authors.lastname: Bozek
authors.affiliation: Sorbonne Universités, UPMC Université Paris 06, Laboratoire de Chimie Physique Matière et Rayonnement, F-75005, Paris, France. CNRS, Laboratoire de Chimie Physique Matière et Rayonnement, F-75005, Paris, France.
authors.forename: Marc
authors.initials: M
authors.lastname: Simon
authors.affiliation: Sorbonne Universités, UPMC Université Paris 06, Laboratoire de Chimie Physique Matière et Rayonnement, F-75005, Paris, France. CNRS, Laboratoire de Chimie Physique Matière et Rayonnement, F-75005, Paris, France.
authors.forename: Tatiana
authors.initials: T
authors.lastname: Marchenko
authors.affiliation: Center for Free-Electron Laser Science (CFEL), DESY, 22607 Hamburg, Germany. Department of Physics, University of Hamburg, 22761 Hamburg, Germany. Center for Ultrafast Imaging, University of Hamburg, 22761 Hamburg, Germany.
authors.forename: Jochen
authors.initials: J
authors.lastname: Küpper
authors.affiliation: Max Planck Advanced Study Group at CFEL, 22607 Hamburg, Germany. Max-Planck-Institut für Medizinische Forschung, 69120 Heidelberg, Germany.
authors.forename: Ilme
authors.initials: I
authors.lastname: Schlichting
authors.affiliation: Physikalisch-Technische Bundesanstalt, 38116 Braunschweig, Germany. Max Planck Advanced Study Group at CFEL, 22607 Hamburg, Germany. Max-Planck-Institut für Kernphysik, 69117 Heidelberg, Germany.
authors.forename: Joachim
authors.initials: J
authors.lastname: Ullrich
authors.affiliation: Linac Coherent Light Source, SLAC National Accelerator Laboratory, 94025 Menlo Park, CA, USA.
authors.forename: Christoph
authors.initials: C
authors.lastname: Bostedt
authors.affiliation: Deutsches Elektronen-Synchrotron (DESY), 22607 Hamburg, Germany. Max Planck Advanced Study Group at CFEL, 22607 Hamburg, Germany. Max-Planck-Institut für Medizinische Forschung, 69120 Heidelberg, Germany.
authors.forename: Daniel
authors.initials: D
authors.lastname: Rolles
authors.affiliation: J. R. Macdonald Laboratory, Department of Physics, Kansas State University, Manhattan, KS 66506, USA. Max Planck Advanced Study Group at CFEL, 22607 Hamburg, Germany. Max-Planck-Institut für Kernphysik, 69117 Heidelberg, Germany. benjamin.erk@desy.de rudenko@phys.ksu.edu.
authors.forename: Artem
authors.initials: A
authors.lastname: Rudenko