title: Coherent electron hole dynamics near a conical intersection.
abstract: The coherent evolution of an electron hole in a photoionized molecule represents an unexplored facet of charge transfer phenomena occurring in complex systems. Using ultrafast extreme ultraviolet spectroscopy, we investigate the real-time dynamics of an electron hole wave packet created near a conical intersection in CO_{2}. We resolve the oscillation of the electron hole density between σ and π character, driven by the coupled bending and asymmetric stretch vibrations of the molecule. We also quantify the mixing between electron hole configurations and find that the wave packet coherence diminishes with time due to thermal dephasing.
authors.affiliation: Department of Physics, University of Arizona, Tucson, Arizona 85721, USA.
authors.forename: Henry
authors.initials: H
authors.lastname: Timmers
authors.affiliation: Center for Free-Electron Laser Science, DESY, Notkestrasse 85, D-22607 Hamburg, Germany and Department of Physics, University of Hamburg, D-20355 Hamburg, Germany.
authors.forename: Zheng
authors.initials: Z
authors.lastname: Li
authors.affiliation: Department of Physics, University of Arizona, Tucson, Arizona 85721, USA.
authors.forename: Niranjan
authors.initials: N
authors.lastname: Shivaram
authors.affiliation: Center for Free-Electron Laser Science, DESY, Notkestrasse 85, D-22607 Hamburg, Germany and Department of Physics, University of Hamburg, D-20355 Hamburg, Germany.
authors.forename: Robin
authors.initials: R
authors.lastname: Santra
authors.affiliation: Center for Free-Electron Laser Science, DESY, Notkestrasse 85, D-22607 Hamburg, Germany.
authors.forename: Oriol
authors.initials: O
authors.lastname: Vendrell
authors.affiliation: Department of Physics, University of Arizona, Tucson, Arizona 85721, USA.
authors.forename: Arvinder
authors.initials: A
authors.lastname: Sandhu
mesh_terms: D002245:Carbon Dioxide / Q000737:chemistry*; D004583:Electrons; D008956:Models, Chemical; D011789:Quantum Theory
chemical_list: D002245:Carbon Dioxide