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Weak covalent bonds drive anionic charge-sharing in clusters. Solvation typically limits polymerisation, restricting the size of bound anions.

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Area of Science:

  • Physical Chemistry
  • Quantum Chemistry
  • Materials Science

Background:

  • Understanding the formation of weak covalent bonds is crucial for cluster chemistry.
  • Anionic charge-sharing interactions influence molecular assembly and material properties.

Purpose of the Study:

  • To investigate the formation of weak covalent bonds leading to anionic charge-sharing dimerisation or polymerisation.
  • To model the interplay between covalent bonding and solvation forces in microscopic clusters.

Main Methods:

  • Utilisation of a coupled-monomers molecular-orbital model.
  • Application of a Hückel-style formalism adapted for weak interactions and solvation.
  • Analysis of inter-monomer orbitals governing charge-sharing phenomena.

Main Results:

  • Coherent charge sharing describes covalent bonding between cluster building blocks.
  • A balance exists between covalent and solvation forces, influencing cluster structure.
  • Solvation effects generally hinder polymerisation, capping the size of anionic clusters.

Conclusions:

  • The coupled-monomers model provides insight into weak covalent bonding and charge sharing.
  • Solvation plays a critical role in limiting the extent of anionic polymerisation in clusters.
  • This work illuminates the fundamental interactions governing the assembly of anionic clusters.