Abstract

Hollow gold nanospheres (HGNs) were excited with ultrashort laser pulses, and the coherent vibrational response was examined using femtosecond time-resolved transient absorption. The results indicated that HGNs support an isotropic mode, resulting in periodic modulation of the surface plasmon differential absorption. Two different categories of coherent acoustic vibrations, which depend on particle dimensions, were observed for HGNs. Further, the vibration launching mechanism was dependent upon the dimensions of the HGN. Coherent vibrations in HGNs characterized by small outer radii (<10 nm) and low cavity-radius-to-outer-shell radius aspect ratios (<0.5) were excited by a direct mechanism, whereas the vibrations observed for the larger particles (>25 nm OR) with higher aspect ratios (>0.5) resulted from an indirect mechanism. These findings may be significant for developing a predictive understanding of nanostructure optical and mechanical properties.

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