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Building clusters atom-by-atom: from local order to global order.

Seyed Mohammad Ghazi1, Shahab Zorriasatein, D G Kanhere

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Summary

Sodium cluster growth exhibits a cyclic order-disorder-order pattern. Global order emerges rapidly, but clusters near N=92 deviate, impacting experimental melting temperatures.

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Area of Science:

  • Physical Chemistry
  • Computational Materials Science
  • Atomic and Molecular Physics

Background:

  • Understanding the growth patterns and structural evolution of sodium clusters (NaN) is crucial for predicting their properties.
  • Previous studies have indicated complex structural behaviors in alkali metal clusters.

Purpose of the Study:

  • To investigate the growth characteristics and structural diversity of sodium clusters (NaN) from N=10 to 147.
  • To identify the relationship between cluster structure, growth patterns, and experimentally observed melting temperatures.

Main Methods:

  • Extensive density functional theory (DFT) calculations were performed.
  • Approximately 13,000 distinct sodium cluster isomers were generated and analyzed.

Main Results:

  • A cyclic order-disorder-order pattern was observed in sodium cluster growth.
  • Disordered clusters with multicentered icosahedral local order bridge ordered structures.
  • Global order in clusters emerges abruptly with the addition of just one or two atoms.
  • Sodium clusters around N=92, an electronically closed shell system, exhibit unique behavior and lack favored icosahedral local order.

Conclusions:

  • The observed growth pattern provides insights into the self-assembly of sodium clusters.
  • The absence of icosahedral local order in clusters around N=92 correlates with experimentally observed lower melting temperatures.