Evolution of Nonlinear Optical Properties: From Gold Atomic Clusters to Plasmonic Nanocrystals

    Authors

    R. Philip; P. Chantharasupawong; H. F. Qian; R. C. Jin;J. Thomas

    Comments

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    Abbreviated Journal Title

    Nano Lett.

    Keywords

    Gold nanoclusters; plasmonic nanocrystals; third-order optical; nonlinearity; optical limiting; PROTECTED GOLD; ABSORPTION SPECTRA; NANOPARTICLES; SIZE; NANOCLUSTERS; AU; COMPLEXES; MOLECULES; DYNAMICS; Chemistry, Multidisciplinary; Chemistry, Physical; Nanoscience &; Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied; Physics, Condensed Matter

    Abstract

    Atomic clusters of metals are an emerging class of extremely interesting materials occupying the intermediate size regime between atoms and nanoparticles. Here we report the nonlinear optical (NLO) characteristics of ultrasmall, atomically precise clusters of gold, which are smaller than the critical size for electronic energy quantization (similar to 2 nm). Our studies reveal remarkable features of the distinct evolution of the optical nonlinearity as the clusters progress in size from the nonplasmonic regime to the plasmonic regime. We ascertain that the smallest atomic clusters do not show saturable absorption at the surface plasmon wavelength of larger gold nanocrystals ( > 2 nm). Consequently, the third-order optical nonlinearity in these ultrasmall gold clusters exhibits a significantly lower threshold for optical power limiting. This limiting efficiency, which is superior to that of plasmonic nanocrystals, is highly beneficial for optical limiting applications.

    Journal Title

    Nano Letters

    Volume

    12

    Issue/Number

    9

    Publication Date

    1-1-2012

    Document Type

    Article

    Language

    English

    First Page

    4661

    Last Page

    4667

    WOS Identifier

    WOS:000308576000041

    ISSN

    1530-6984

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