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Modulating Electronic Coupling Using O- and S-donor Linkers.

F Albert Cotton1, Zhong Li, Chun Y Liu

  • 1Department of Chemistry and Laboratory for Molecular Structure and Bonding, P.O. Box 3012, Texas A&M University, College Station, Texas 77842-3012, USA.

Inorganic Chemistry
|August 21, 2007
PubMed
Summary
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Replacing oxygen with sulfur in dimolybdenum compounds enhances electronic coupling, leading to intense charge transfer bands and facilitating electron hopping pathways. This structural modification is key for advanced electronic applications.

Area of Science:

  • Inorganic Chemistry
  • Materials Science
  • Electrochemistry

Background:

  • Dimolybdenum compounds with formamidinate ligands are known for their unique electronic properties.
  • Investigating the impact of linker modifications on electronic communication between metal centers is crucial for developing new materials.

Purpose of the Study:

  • To synthesize and characterize dimolybdenum compounds linked by oxamidate and dithiooxamidate.
  • To evaluate the effect of replacing oxygen with sulfur in the linker on electronic coupling and charge transfer properties.

Main Methods:

  • X-ray crystallography for structural determination.
  • Molecular mechanics and Density Functional Theory (DFT) calculations for conformational analysis and electronic structure.
  • Electrochemical measurements (cyclic voltammetry) to determine electronic coupling.

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  • UV-Vis spectroscopy to study electronic transitions.

    • Main Results:

    • Isomorphous structures of dimolybdenum units connected by oxamidate and dithiooxamidate linkers were determined.
    • The dithiooxamidate linker significantly enhanced electronic coupling between dimolybdenum units (407 mV vs 204 mV).
    • The dithiooxamidate compound exhibited an intense low-energy metal-to-ligand charge transfer band at 600 nm, unlike the oxamidate compound.

    Conclusions:

    • The replacement of oxygen with sulfur atoms in the linker facilitates stronger electronic coupling and facilitates electron hopping pathways.
    • The sulfur atoms in the dithiooxamidate linker lower the pi* orbital energy, enabling dpi-ddelta interactions and enhancing electronic communication.
    • These findings highlight the potential of sulfur-containing linkers in designing advanced dimolybdenum-based electronic materials.