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Trapping a Photoelectron behind a Repulsive Coulomb Barrier in Solution.

Meixin Cheng1, Nicolás Rivas1, Su Ji Lim1

  • 1Department of Chemistry, and Waterloo Institute for Nanotechnology , University of Waterloo , 200 University Avenue W. , Waterloo , ON N2L 3G1 , Canada.

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Multiply charged anions (MCAs) in water, like B12F12(2-), possess a repulsive Coulomb barrier (RCB). This barrier prevents electron ejection, even with strong Coulomb repulsion, stabilizing the anion in solution.

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Area of Science:

  • Physical Chemistry
  • Chemical Physics
  • Spectroscopy

Background:

  • Multiply charged anions (MCAs) exhibit unique photophysics and solvent interactions.
  • Aqueous MCAs like SO4(2-) and PO4(3-) often undergo electron detachment or fragmentation in the gas phase due to Coulomb repulsion.
  • Anions typically have low photodetachment thresholds and can eject electrons into solvents via charge-transfer-to-solvent (CTTS) states.

Purpose of the Study:

  • To investigate the photophysics of the aqueous B12F12(2-) dianion.
  • To provide spectroscopic evidence for a repulsive Coulomb barrier (RCB) in aqueous MCAs.
  • To understand the behavior of photoexcited electrons in multiply charged anions in solution.

Main Methods:

  • Spectroscopic experiments were conducted on the aqueous B12F12(2-) dianion.
  • Theoretical studies were performed to analyze the potential energy landscape.
  • Ultrafast electron dynamics were probed to observe electron ejection behavior.

Main Results:

  • Spectroscopic evidence confirmed the existence of an RCB for the aqueous B12F12(2-) dianion.
  • The RCB was found to block the ejection of "CTTS-like" electrons.
  • Experimental and theoretical data showed that the photoexcited electron remains localized near the B12F12(-•) core, despite Coulomb repulsion.

Conclusions:

  • The repulsive Coulomb barrier (RCB) is not limited to the gas phase but extends to the liquid phase for aqueous MCAs.
  • This RCB phenomenon influences the dielectric behavior of confined water.
  • The findings challenge the typical understanding of electron ejection from anions in solution.