Spectroscopy of vibrational modes in metal nanoshells

We study the spectrum of vibrational modes in metal nanoparticles with a dielectric core. Vibrational modes are excited by the rapid heating of the particle lattice that takes place after laser excitation, and can be monitored by means of pump-probe spectroscopy as coherent oscillations of transient optical spectra. In nanoshells, the presence of two metal surfaces results in a substantially different energy spectrum of acoustic vibrations than for solid particles. We calculated the energy spectrum as well as the damping of nanoshell vibrational modes. The oscillator strength of fundamental breathing mode is larger than that in solid nanoparticles. At the same time, in very thin nanoshells, the fundamental mode is overdamped due to instantaneous energy transfer to the surrounding medium

Continuum limit of amorphous elastic bodies: A finite-size study of low frequency harmonic vibrations

The approach of the elastic continuum limit in small amorphous bodies formed by weakly polydisperse Lennard-Jones beads is investigated in a systematic finite-size study. We show that classical continuum elasticity breaks down when the wavelength of the sollicitation is smaller than a characteristic length of approximately 30 molecular sizes. Due to this surprisingly large effect ensembles containing up to N=40,000 particles have been required in two dimensions to yield a convincing match with the classical continuum predictions for the eigenfrequency spectrum of disk-shaped aggregates and periodic bulk systems. The existence of an effective length scale \xi is confirmed by the analysis of the (non-gaussian) noisy part of the low frequency vibrational eigenmodes. Moreover, we relate it to the {\em non-affine} part of the displacement fields under imposed elongation and shear. Similar correlations (vortices) are indeed observed on distances up to \xi~30 particle sizes.Comment: 28 pages, 13 figures, 3 table

Femtosecond optical investigation of electron-lattice interactions in an ensemble and a single metal nanoparticle

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The coalescence of supported gold nanoparticles induced by nanosecond laser irradiation

Gold nanoparticles supported on a quartz substrate are fabricated by e-beam lithography and subjected to nanosecond laser irradiation to induce coalescence. In combination with ex-situ scanning electron microscopy and optical extinction spectra, transmission is monitored in-situ to determine the characteristic coalescence time, the threshold fluence for the onset of coalescence and the produced particle morphology. Parallel molecular dynamics simulation is employed and shown to reasonably predict the coalescence time, thus explaining the experimental results