Coherent electron hole dynamics near a conical intersection

Henry Timmers, Zheng Li, Niranjan Shivaram, Robin Santra, Oriol Vendrell, Arvinder Singh Sandhu

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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.

Original languageEnglish (US)
Article number113003
JournalPhysical Review Letters
Volume113
Issue number11
DOIs
Publication statusPublished - Sep 12 2014

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ASJC Scopus subject areas

  • Physics and Astronomy(all)
  • Medicine(all)

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