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Femtosecond X-ray Spectroscopy Directly Quantifies Transient Excited-State Mixed Valency.

Chelsea Liekhus-Schmaltz1, Zachary W Fox1, Amity Andersen2

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|January 5, 2022
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Summary
This summary is machine-generated.

Measuring charge delocalization in photoexcited molecular complexes is difficult. This study quantifies evolving charge distribution in iron-ruthenium complexes using X-ray spectroscopy and computational methods.

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Area of Science:

  • Photochemistry
  • Physical Chemistry
  • Spectroscopy

Background:

  • Quantifying charge delocalization in short-lived photoexcited states of molecular complexes in solution is experimentally challenging.
  • Femtosecond experimental probes are required for time-evolving electron transfer studies.

Purpose of the Study:

  • To quantify the evolving valence hole charge distribution in the photoexcited charge transfer state of a mixed valence bimetallic iron-ruthenium complex in water.
  • To establish a spectroscopic ruler for quantifying excited-state valency in solvated complexes.

Main Methods:

  • Combining femtosecond X-ray spectroscopy measurements with time-dependent density functional theory (TD-DFT) calculations.
  • Investigating the excited-state dynamics of [(CN)5FeIIcyanoRuIII(NH3)5]- in water.

Main Results:

  • Estimated valence hole charge accumulated at the Fe atom to be 0.6 ± 0.2.
  • Observed excited-state metal-to-metal charge transfer on an approximately 60 fs timescale.

Conclusions:

  • The combined experimental and computational approach successfully quantifies excited-state valency.
  • This method provides a valuable tool for studying ultrafast charge dynamics in solvated complexes.