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Centered germanium clusters (Ge@Ge₁₀) are energetically competitive with empty clusters for cationic species. DFT calculations reveal these structures form by inserting germanium ions into smaller germanium clusters.

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Area of Science:

  • Computational chemistry
  • Materials science
  • Solid-state physics

Background:

  • Investigating germanium clusters is crucial for understanding their unique electronic and structural properties.
  • Previous studies focused on empty 11-vertex Ge₁₁(z) clusters, leaving centered structures less explored.

Purpose of the Study:

  • To investigate the structures and energetics of centered 10-vertex Ge@Ge₁₀(z) clusters.
  • To compare the stability of centered germanium clusters with isomeric empty germanium clusters.
  • To explore the influence of charge state (z = -4, -2, 0, +2, +4) on cluster stability.

Main Methods:

  • Density functional theory (DFT) calculations were employed to determine cluster structures and energies.
  • Systematic investigation of centered 10-vertex Ge@Ge₁₀(z) clusters across various charge states.
  • Comparison of calculated energetics with previously reported data for empty Ge₁₁(z) clusters.

Main Results:

  • Centered Ge@Ge₁₀(z) structures are energetically competitive with empty Ge₁₁(z) clusters for cationic species (z = +2, +4).
  • These centered structures can be formed by inserting a Ge⁴⁺ ion into lower-energy empty 10-vertex Ge₁₀(z-4) clusters.
  • The lowest energy Ge@Ge₁₀²⁺ structure features a D(4d) bicapped square antiprism, consistent with Wade-Mingos rules.
  • Centered structures for neutral and dianionic germanium clusters were found but are less stable than their empty counterparts.

Conclusions:

  • Centered germanium clusters, particularly cationic ones, represent stable structural motifs.
  • The formation of centered clusters offers a new perspective on germanium cluster isomerism.
  • DFT provides a reliable method for predicting the stability and structure of germanium clusters.