Femtosecond Photoelectron Imaging of Aligned Polyanions: Probing Molecular Dynamics through the Electron−Anion Coulomb Repulsion

Horke, D.A.; Chatterley, A.S.; Verlet, J.R.R.

Abstract

The first time-resolved photoelectron imaging study of a polyanion is presented. Using the alignment induced through resonance excitation, the photoelectron angular distributions can be qualitatively understood in terms of the position of localized excess charges on the molecular skeleton, which influence the photoemission dynamics. Pump–probe experiments are used to demonstrate that the photoelectron angular distribution is also sensitive to molecular dynamics. This is shown here for the rotational dynamics of a polyanion, in which the photoelectron anisotropy tracks the rotational coherence as it dephases. The methodology can in principle be applied to general molecular dynamics in large polyanions, providing a new route to studying ultrafast structural dynamics in complex gas-phase systems.

Citation

Horke, D., Chatterley, A., & Verlet, J. (2012). Femtosecond Photoelectron Imaging of Aligned Polyanions: Probing Molecular Dynamics through the Electron−Anion Coulomb Repulsion. Journal of Physical Chemistry Letters, 3(7), 834-838. https://doi.org/10.1021/jz3000933

• Journal Article Type: Article
• Acceptance Date: Mar 6, 2012
• Publication Date: Apr 5, 2012
• Deposit Date: May 15, 2013
• Publicly Available Date: Feb 5, 2016
• Journal: Journal of Physical Chemistry Letters
• Electronic ISSN: 1948-7185
• Publisher: American Chemical Society
• Peer Reviewed: Peer Reviewed
• Volume: 3
• Issue: 7
• Pages: 834-838
• DOI: https://doi.org/10.1021/jz3000933
• Public URL: https://durham-repository.worktribe.com/output/1453226