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Covalent Group IV Atomic Clusters.

W L Brown, R R Freeman, K Raghavachari

    Science (New York, N.Y.)
    |February 20, 1987
    PubMed
    Summary
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    Researchers studied atomic clusters of carbon, silicon, and germanium to understand their transition from molecules to solids. Fragmentation patterns reveal unique behaviors for carbon clusters compared to silicon and germanium clusters.

    Area of Science:

    • Materials Science
    • Physical Chemistry
    • Nanotechnology

    Background:

    • Atomic clusters bridge the gap between molecular and solid-state physics.
    • Group IV elements (carbon, silicon, germanium) exhibit diverse bonding and solid-state properties.
    • Understanding cluster stability and structure is key to materials design.

    Purpose of the Study:

    • Investigate the transition from atomic clusters to crystalline solids for group IV elements.
    • Determine the relative stability and fragmentation patterns of carbon, silicon, and germanium clusters.
    • Compare experimental findings with theoretical calculations for cluster structures.

    Main Methods:

    • Formation of mass-selected atomic cluster ions using pulsed laser techniques.
    • Identification of clusters via time-of-flight mass spectrometry.

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  • Laser photoexcitation to study cluster stability and fragmentation pathways.

    • Main Results:

    • Carbon clusters (C(n)(+)) exhibit distinct fragmentation, often losing C(3).
    • Silicon (Si(n)(+)) and germanium (Ge(n)(+)) clusters show preferential fragmentation to "magic" clusters like Si(4)(+), Si(6)(+), and Si(10)(+).
    • Theoretical calculations align with experimental data, revealing compact structures for silicon clusters and a shift from linear to cyclic structures for carbon clusters with increasing size.

    Conclusions:

    • Fragmentation behaviors differ significantly between carbon and silicon/germanium atomic clusters.
    • Theoretical models accurately predict the structure and stability of small silicon and carbon clusters.
    • Small silicon clusters possess unique compact structures, distinct from bulk crystal fragments.