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Computation of Atmospheric Concentrations of Molecular Clusters from ab initio Thermochemistry
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Structural evolution of medium-sized Pd(n) (n=15-25) clusters from density functional theory.

Hualei Zhang1, Dongxu Tian, Jijun Zhao

  • 1School of Physics and Optoelectronic Technology and College of Advanced Science and Technology, Dalian University of Technology, Dalian 116024, China. zhaojj@dlut.edu.cn

The Journal of Chemical Physics
|December 3, 2008
PubMed
Summary

Medium-sized palladium clusters (Pd(n), n=15-25) were studied for structural motifs. The Pd(19) octahedron with an fcc-like structure shows particular stability, dominating cluster growth.

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Area of Science:

  • * Computational materials science and condensed matter physics.
  • * Investigating the structural and electronic properties of medium-sized metal clusters.

Background:

  • * Understanding the structure-property relationships in transition metal clusters is crucial for catalysis and materials design.
  • * Medium-sized clusters (n=15-25) often exhibit complex structural transitions and unique electronic behaviors.

Purpose of the Study:

  • * To explore and identify stable structural motifs for palladium clusters (Pd(n), n=15-25).
  • * To investigate the correlation between geometric structure and electronic properties.
  • * To determine size-dependent stability trends in these palladium clusters.

Main Methods:

  • * Empirical genetic algorithm search for generating potential cluster structures.
  • * Spin-polarized density functional theory (DFT) calculations for electronic structure and energy optimization.
  • * Analysis of size-dependent properties and geometric-electronic correlations.

Main Results:

  • * Identified four primary structural motifs: fcc-like, decahedron-based, icosahedron-based, and prolate ellipsoid-based.
  • * Pd(19) with an fcc-like octahedron structure dominates the growth pathway for clusters (n=15-23).
  • * Energetically favorable structures for larger clusters (Pd(24), Pd(25)) include prolate ellipsoid and triple decahedra.

Conclusions:

  • * The Pd(19) cluster with an fcc-like octahedron structure represents a particularly stable motif.
  • * Cluster geometry significantly influences electronic properties and stability.
  • * Structural transitions occur with increasing cluster size, favoring different motifs at Pd(24) and Pd(25).