Breathing Mode Dynamics and Elastic Properties of Gold Nanoparticles

Charles F. Vardeman II, Patrick F. Conforti, Megan M. Sprague, and J. Daniel Gezelter*
Department of Chemistry and Biochemistry, University of Notre Dame, Notre Dame, Indiana 46556
J. Phys. Chem. B, 2005, 109 (35), pp 16695–16699
DOI: 10.1021/jp051575r
Publication Date (Web): August 12, 2005
Copyright © 2005 American Chemical Society

Abstract

We present calculations of the bulk modulus, heat capacity, and the period of the breathing mode for spherical nanoparticles following excitation by ultrafast laser pulses. The bulk modulus and heat capacities both exhibit clear transitions upon bulk melting of the particles. Equilibrium calculations of the heat capacity show that the melting transition is sharper and occurs at a lower temperature than one would observe from an ultrafast experiment. We also observe an intriguing splitting in the low-frequency spectra of the nanoparticles and analyze this splitting in terms of Lamb's classical theory of elastic spheres. We conclude that the particles either (1) melt during the observation period following laser excitation or (2) melt an outer shell while maintaining a crystalline core. Both mechanisms for melting are commensurate with our observations.

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History

  • Published In Issue September 08, 2005
  • Received March 28, 2005

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