Time-resolved spectroscopy of silver nanocubes: Observation and assignment of coherently excited vibrational modes

被引:71
作者
Petrova, Hristina [1 ]
Lin, Chien-Hua
de Liejer, Suzanna
Hu, Min
McLellan, Joseph M.
Siekkinen, Andrew R.
Wiley, Benjamin J.
Marquez, Manuel
Xia, Younan
Sader, John E.
Hartland, Gregory V.
机构
[1] Univ Notre Dame, Dept Chem & Biochem, Notre Dame, IN 46556 USA
[2] Univ Melbourne, Dept Math & Stat, Melbourne, Vic 3010, Australia
[3] Univ Washington, Dept Chem, Seattle, WA 98195 USA
[4] NIST, NCTCN Ctr, Phys & Chem Properties Div, Gaithersburg, MD 20899 USA
[5] Univ Washington, Dept Chem, Seattle, WA 98195 USA
基金
美国国家科学基金会; 澳大利亚研究理事会;
关键词
D O I
10.1063/1.2672907
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The response of single crystal, cubic silver particles to ultrafast laser-induced heating has been examined experimentally and theoretically. The transient absorption traces display clear modulations due to coherently excited vibrational modes. Nanocube samples with edge lengths smaller than 50 nm show a single modulation, whereas samples larger than 50 nm show two vibrational modes. The results are compared to finite element calculations, where the cubes are modeled as having cubic crystal symmetry with the principal axes parallel to the sides of the particle. The action of the laser pulse is treated in two ways, first, as creating a uniform initial strain. In this case the predominant mode excited is the breathing mode. The period of this mode is in reasonable agreement with the vibrational periods measured for the smaller cubes and with the higher frequency modulation observed for the larger cubes. A nonuniform initial strain is also considered, which could arise from nonuniform heating for particles larger than the optical skin depth of the metal. In this case the predominant mode excited is a nontotally symmetric mode. The calculated periods from this analysis are in reasonable agreement with the lower frequency modulations observed for the larger samples. The results from this study show that, to within the accuracy of these measurements, the elastic constants of cubic silver nanoparticles are the same as bulk silver.
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页数:8
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