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Electronic Coupling in [Mo2]-Bridge-[Mo2] Systems with Twisted Bridges.

Hong Li Zhang1, Guang Yuan Zhu1, Gangyi Wang1

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Inorganic Chemistry
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The study synthesized two Mo2 dimers to investigate how bridge conformation affects electronic coupling in donor-bridge-acceptor systems. Results show distinct optical behaviors and electronic coupling classifications (Class I and Class II) based on bridge geometry.

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Area of Science:

  • Coordination Chemistry
  • Supramolecular Chemistry
  • Photochemistry

Background:

  • Donor-bridge-acceptor (DBA) triad systems are crucial for understanding electron transfer processes.
  • The conformation of the bridging ligand significantly influences electronic coupling and charge transfer.
  • Previous studies on phenylene-bridged Mo2 dimers established baseline electronic coupling behaviors.

Purpose of the Study:

  • To synthesize and characterize novel Mo2 dimers with distinct bridge conformations.
  • To evaluate the impact of varying bridge geometry on electronic coupling in mixed-valence (MV) states.
  • To elucidate the roles of through-space electrostatic interactions and through-bond electron resonance.

Main Methods:

  • Synthesis and structural characterization of two new Mo2 dimer complexes ([Mo2(DAniF)3]2[μ-1,4-{C(O)NH}2-Naph] (1) and [Mo2(DAniF)3]2[μ-1,4-(CS2)2-2,5-Me2C6H2] (2)).
  • Generation of mixed-valence (MV) species via single-electron oxidation.
  • Optical spectroscopy (UV-Vis-NIR) to observe intervalence charge transfer (IVCT) bands.
  • Analysis using superexchange formalism and Hush model for electronic coupling quantification.

Main Results:

  • Complexes 1 and 2 exhibit large dihedral angles (>60°) in their bridge conformations, differing from planar phenylene analogues.
  • MV species 1(+) shows no IVCT band (Class I, electronically uncoupled), while MV species 2(+) displays a weak IVCT band (Class II, weakly coupled, Hab = 220 cm(-1)).
  • This contrasts with previously studied phenylene-bridged analogues, demonstrating a transition from Class I to Class II-III borderline behavior by altering bridge topology.

Conclusions:

  • Bridge conformation critically dictates the electronic coupling strength in these Mo2 DBA systems.
  • The observed differences in IVCT bands and Robin-Day classifications highlight the influence of geometric topology.
  • The study provides insights into the interplay of electrostatic and resonance effects governing electronic communication in molecular systems.