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Time- and Temperature-Resolved Triplet Dynamics in Tungsten Iodide Clusters.

Philipp Frech1, Wolfgang Leis2, Florian Pachel3

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Tungsten iodide clusters show rapid intersystem crossing to triplet states. A relativistic model explains their excited-state dynamics, differing from previous molybdenum cluster studies.

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Area of Science:

  • Inorganic Chemistry
  • Photochemistry
  • Materials Science

Background:

  • Tungsten iodide clusters are promising materials for photochemical applications.
  • Understanding their excited-state dynamics is crucial for designing new functional materials.

Purpose of the Study:

  • To investigate the excited-state dynamics of tungsten iodide clusters.
  • To explore the deactivation pathways of triplet states.
  • To compare the behavior of tungsten clusters with molybdenum clusters.

Main Methods:

  • Ultrafast transient absorption spectroscopy (200 fs to 400 μs).
  • Temperature-dependent emission spectroscopy (4 K to 340 K).
  • Time-dependent density functional theory (TD-DFT) calculations.

Main Results:

  • Rapid intersystem crossing (< 6 ps) populates triplet states.
  • Triplet states deactivate via emission or bimolecular quenching with oxygen.
  • Temperature-dependent emission aligns with a three-sublevel model.
  • No experimental splitting of lowest triplet states observed, unlike molybdenum clusters.
  • TD-DFT reveals significant excited-state geometrical distortions.

Conclusions:

  • A relativistic model with three thermally accessible geometries, each with three triplet sublevels, is proposed.
  • Group-theoretical models alone are insufficient to describe the observed dynamics.
  • Excited-state distortions play a key role in the photophysics of these tungsten clusters.