Coherent Electron Hole Dynamics Near a Conical Intersection

Henry Timmers, Zheng Li, Niranjan Shivaram, Robin Santra, Oriol Vendrell, and Arvinder Sandhu
Phys. Rev. Lett. 113, 113003 – Published 12 September 2014
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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 CO2. 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.

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  • Received 24 June 2014

DOI:https://doi.org/10.1103/PhysRevLett.113.113003

© 2014 American Physical Society

Authors & Affiliations

Henry Timmers1, Zheng Li2,3, Niranjan Shivaram1, Robin Santra2,3, Oriol Vendrell2, and Arvinder Sandhu1,*

  • 1Department of Physics, University of Arizona, Tucson, Arizona 85721, USA
  • 2Center for Free-Electron Laser Science, DESY, Notkestrasse 85, D-22607 Hamburg, Germany
  • 3Department of Physics, University of Hamburg, D-20355 Hamburg, Germany

  • *sandhu@physics.arizona.edu

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Vol. 113, Iss. 11 — 12 September 2014

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