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Electronically Coupled, Cofacially Linked, Hypervalent Antimony(V) Porphyrin Homodimer: Synthesis, Spectroscopy, and

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A new cofacial homodimer of hypervalent antimony(V) porphyrins was synthesized. This stable structure exhibits significant exciton coupling, challenging traditional dipole-dipole models for excited-state properties.

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Area of Science:

  • Supramolecular Chemistry
  • Organometallic Chemistry
  • Photochemistry

Background:

  • Cofacial porphyrin dimers are crucial for understanding energy transfer and electron transfer processes.
  • Hypervalent main group elements, like antimony, offer unique electronic properties for porphyrin chemistry.

Purpose of the Study:

  • To synthesize and characterize a covalently linked cofacial homodimer of hypervalent antimony(V) porphyrins.
  • To investigate the electronic communication and excited-state properties of the dimer.
  • To explore the role of antimony in promoting exciton coupling.

Main Methods:

  • Synthesis of antimony(V) porphyrin homodimer.
  • X-ray crystallography for structural determination.
  • Density Functional Theory (DFT) calculations.
  • Optical spectroscopy (UV-Vis absorption).
  • Femtosecond and nanosecond transient absorption spectroscopy.
  • Time-resolved electron paramagnetic resonance (TREPR).

Main Results:

  • A stable cofacial homodimer linked by an -OCH2O- bridge was successfully synthesized.
  • The dimer exhibits strong exciton coupling, evidenced by delocalized HOMO/LUMO and spectral shifts.
  • DFT and optical data suggest H-type exciton coupling, but the dipole-dipole model is insufficient.
  • The triplet state is localized on a single porphyrin, consistent with weak triplet-triplet coupling.
  • Antimony(V) plays a key role in promoting exciton coupling in these cofacial porphyrin systems.

Conclusions:

  • The synthesized antimony(V) porphyrin homodimer demonstrates robust exciton coupling.
  • The study highlights the limitations of the dipole-dipole model for describing excited-state behavior in such systems.
  • Hypervalent antimony is crucial for facilitating exciton coupling in cofacial porphyrin dimers.