Coherent Electron Hole Dynamics Near a Conical Intersection

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

doi:10.1103/PhysRevLett.113.113003

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Coherent Electron Hole Dynamics Near a Conical Intersection

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Li, Zheng
Center for Free-Electron Laser Science, DESY, Notkestrasse 85, D-22607 Hamburg, Germany;
Department of Physics, University of Hamburg, D-20355 Hamburg, Germany;
International Max Planck Research School for Ultrafast Imaging & Structural Dynamics (IMPRS-UFAST), Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;

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http://dx.doi.org/10.1103/PhysRevLett.113.113003
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引用

Timmers, H., Li, Z., Shivaram, N., Santra, R., Vendrell, O., & Sandhu, A. (2014). Coherent Electron Hole Dynamics Near a Conical Intersection. Physical Review Letters, 113(11):. doi:10.1103/PhysRevLett.113.113003.

引用: https://hdl.handle.net/11858/00-001M-0000-002A-F473-B

要旨

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.