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Trapping a Photoelectron behind a Repulsive Coulomb Barrier in Solution

  • Meixin Cheng
    Meixin Cheng
    Department of Chemistry, and Waterloo Institute for Nanotechnology, University of Waterloo, 200 University Avenue W., Waterloo, ON N2L 3G1, Canada
    More by Meixin Cheng
  • Nicolás Rivas
    Nicolás Rivas
    Department of Chemistry, and Waterloo Institute for Nanotechnology, University of Waterloo, 200 University Avenue W., Waterloo, ON N2L 3G1, Canada
  • Su Ji Lim
    Su Ji Lim
    Department of Chemistry, and Waterloo Institute for Nanotechnology, University of Waterloo, 200 University Avenue W., Waterloo, ON N2L 3G1, Canada
    More by Su Ji Lim
  • Kostyantyn Pichugin
    Kostyantyn Pichugin
    Department of Chemistry, and Waterloo Institute for Nanotechnology, University of Waterloo, 200 University Avenue W., Waterloo, ON N2L 3G1, Canada
  • Ariel A. Petruk
    Ariel A. Petruk
    Department of Chemistry, and Waterloo Institute for Nanotechnology, University of Waterloo, 200 University Avenue W., Waterloo, ON N2L 3G1, Canada
  • Anna Klinkova
    Anna Klinkova
    Department of Chemistry, and Waterloo Institute for Nanotechnology, University of Waterloo, 200 University Avenue W., Waterloo, ON N2L 3G1, Canada
  • Rodney Smith
    Rodney Smith
    Department of Chemistry, and Waterloo Institute for Nanotechnology, University of Waterloo, 200 University Avenue W., Waterloo, ON N2L 3G1, Canada
    More by Rodney Smith
  • W. Scott Hopkins*
    W. Scott Hopkins
    Department of Chemistry, and Waterloo Institute for Nanotechnology, University of Waterloo, 200 University Avenue W., Waterloo, ON N2L 3G1, Canada
    *E-mail: [email protected]
  • , and 
  • Germán Sciaini*
    Germán Sciaini
    Department of Chemistry, and Waterloo Institute for Nanotechnology, University of Waterloo, 200 University Avenue W., Waterloo, ON N2L 3G1, Canada
    *E-mail: [email protected]
Cite this: J. Phys. Chem. Lett. 2019, 10, 19, 5742–5747
Publication Date (Web):September 9, 2019
https://doi.org/10.1021/acs.jpclett.9b01712
Copyright © 2019 American Chemical Society

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    Abstract

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    Multiply charged anions (MCAs) display unique photophysics and solvent-stabilizing effects. Well-known aqueous species such as SO42– and PO43– experience spontaneous electron detachment or charge-separation fragmentation in the gas phase owing to the strong Coulomb repulsion arising from the excess of negative charge. Thus, anions often present low photodetachment thresholds and the ability to quickly eject electrons into the solvent via charge-transfer-to-solvent (CTTS) states. Here, we report spectroscopic evidence for the existence of a repulsive Coulomb barrier (RCB) that blocks the ejection of “CTTS-like” electrons of the aqueous B12F122– dianion. Our spectroscopic experimental and theoretical studies indicate that despite the exerted Coulomb repulsion by the nascent radical monoanion B12F12–•aq, the photoexcited electron remains about the B12F12–• core. The RCB is an established feature of the potential energy landscape of MCAs in vacuo, which seems to extend to the liquid phase highlighting recent observations about the dielectric behavior of confined water.

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    Cited By

    This article is cited by 1 publications.

    1. Yuriko Tasaka, Katsunosuke Nakamura, Sami Malola, Keisuke Hirata, Kuenhee Kim, Kiichirou Koyasu, Hannu Häkkinen, Tatsuya Tsukuda. Electron Binding in a Superatom with a Repulsive Coulomb Barrier: The Case of [Ag44(SC6H3F2)30]4– in the Gas Phase. The Journal of Physical Chemistry Letters 2020, 11 (8) , 3069-3074. https://doi.org/10.1021/acs.jpclett.0c00786