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Vibrational Coherence Spectroscopy Identifies Ultrafast Branching in an Iron(II) Sensitizer.

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N-heterocyclic carbene ligands enhance iron(II) complex lifetimes for photocatalysis. However, the triplet metal-centered state (3MC) acts as a deactivation pathway, limiting applications.

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Area of Science:

  • Inorganic Chemistry
  • Photochemistry
  • Spectroscopy

Background:

  • N-heterocyclic carbene ligands extend metal-to-ligand charge transfer (MLCT) state lifetimes in iron(II) complexes.
  • These complexes show promise for photocatalysis, but their efficiency is limited by excited-state deactivation pathways.

Purpose of the Study:

  • Investigate the role of the triplet metal-centered (3MC) state in the deactivation of MLCT states in an iron(II) sensitizer.
  • Elucidate the deactivation mechanisms impacting the excited-state lifetimes.

Main Methods:

  • Utilized time-resolved vibrational spectroscopy to probe excited-state dynamics.
  • Employed quantum chemical calculations to assign vibrational modes and understand electronic states.

Main Results:

  • Identified two distinct Fe-L breathing vibrations below 150 cm-1.
  • Assigned these vibrations to the 3MC and 3MLCT states using theoretical calculations.
  • Demonstrated ultrafast branching upon excitation, forming both the long-lived 3MLCT and the 3MC state.

Conclusions:

  • The triplet metal-centered (3MC) state is an additional deactivation channel for the excited-state manifold.
  • Understanding and controlling the 3MC state is crucial for optimizing iron(II) photocatalysts.