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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.

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


Authors

D.A. Horke

A.S. Chatterley



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 Mar 28, 2024
Journal Journal of Physical Chemistry Letters
Publisher American Chemical Society
Peer Reviewed Peer Reviewed
Volume 3
Issue 7
Pages 834-838
DOI https://doi.org/10.1021/jz3000933

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Copyright Statement
This document is the Accepted Manuscript version of a Published Work that appeared in final form in The Journal of Physical Chemistry Letters, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see http://dx.doi.org/10.1021/jz3000933.




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