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Rapid excited-state structural reorganization captured by pulsed X-rays.

Lin X Chen1, Guy Jennings, Tao Liu

  • 1Chemistry Division and Materials Science Division, Argonne National Laboratory, Argonne, IL 60439, USA. lchen@anl.gov

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Researchers used X-rays to characterize a photoluminescent excited state of a copper complex in solution. This study provides the first X-ray data of a molecular excited state in a fluid environment on the nanosecond timescale.

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Area of Science:

  • Photochemistry
  • Inorganic Chemistry
  • X-ray Spectroscopy

Background:

  • Metal-to-ligand charge-transfer (MLCT) excited states are crucial in photochemistry.
  • Understanding the structural dynamics of these states in solution is challenging.
  • Previous studies lacked direct structural information on transient excited states in fluid media.

Purpose of the Study:

  • To structurally characterize the nanosecond MLCT excited state of [Cu(I)(dmp)2](BArF) in toluene.
  • To investigate the geometric changes occurring upon photoexcitation.
  • To provide the first X-ray structural data of a molecular excited state in solution.

Main Methods:

  • Visible light photoexcitation of [Cu(I)(dmp)2](BArF).
  • Time-resolved X-ray absorption spectroscopy using pulsed X-rays.
  • Analysis of X-ray data to determine structural parameters of the excited state.

Main Results:

  • A photoluminescent MLCT excited state with a lifetime of 98 ± 5 ns was observed.
  • The excited state features a five-coordinate copper center (Cu(II) in a Cu(I) geometry) with increased Cu-N bond lengths (average increase of 0.07 Å).
  • The coordination geometry changes to a distorted trigonal bipyramid.

Conclusions:

  • The transiently formed five-coordinate MLCT state is photoluminescent, indicating distinct geometries for absorptive and emissive states.
  • This work presents the first X-ray characterization of a molecular excited state in fluid solution on the nanosecond timescale.
  • The findings offer new insights into the structural dynamics of excited states in solution.