In glass, starting from a dependence of the Angells fragility on the Poisson ratio [V. N. Novikov and A. P. Sokolov, Nature 431, 961 (2004)], and a dependence of the Poisson ratio on the atomic packing density [G. N. Greaves et al., Nat. Mater. 10, 8
23 (2011)], we propose that the heterogeneities are predominantly density fluctuations in strong glasses (lower Poisson ratio) and shear elasticity fluctuations in fragile glasses (higher Poisson ratio). Because the excess of low-frequency vibration modes in comparison with the Debye regime (boson peak) is strongly connected to these fluctuations, we propose that they are breathing-like (with change of volume) in strong glasses and shear-like (without change of volume) in fragile glasses. As a verification, it is confirmed that the excess modes in the strong silica glass are predominantly breathing-like. Moreover, it is shown that the excess breathing-like modes in a strong polymeric glass are replaced by shear-like modes under hydrostatic pressure as the glass becomes more compact.
Low-frequency Raman scattering spectra are presented for gold nanocrystals with diameters 3.5 and 13 nm. The frequencies of the Raman peaks but also their number are shown to vary with the nanocrystal size. These results are analyzed using both the c
ontinuous elastic medium approximation and an atomistic approach. We show that the number of atoms in the nanocrystal determines an upper limit of the number of observable Raman features. The frequency range in which the continuous elastic medium approximation is valid is defined by comparison with the calculations based on the atomistic approach.
The purpose of this work is to calculate the vibrational modes of an elastically anisotropic sphere embedded in an isotropic matrix. This has important application to understanding the spectra of low-frequency Raman scattering from nanoparticles embe
dded in a glass matrix. First some low frequency vibrational modes of a free cubically elastic sphere are found to be nearly independent of one combination of elastic constants. This is then exploited to obtain an isotropic approximation for these modes which enables to take into account the surrounding isotropic matrix. This method is then used to quantatively explain recent spectra of gold and copper nanocrystals in glasses.
High resolution low frequency Raman scattering measurements from embedded AgAu nanoparticles unveil efficient scattering by harmonics of both the quadrupolar and the spherical modes. Comparing the experimental data with theoretical calculations that
account for both the embedding medium and the resonant Raman process enables a very complete description of the observed multiple components in terms of harmonics of both the quadrupolar and spherical modes, with a dominating Raman response from the former ones. It is found that only selected harmonics of the quadrupolar mode contribute significantly to the Raman spectra in agreement with earlier theoretical predictions.
The inelastic scattering of neutrons by nanoparticles due to acoustic vibrational modes (energy below 10 meV) confined in nanoparticles is calculated using the Zemach-Glauber formalism. Such vibrational modes are commonly observed by light scattering
techniques (Brillouin or low-frequency Raman scattering). We also report high resolution inelastic neutron scattering measurements for anatase TiO2 nanoparticles in a loose powder. Factors enabling the observation of such vibrations are discussed. These include a narrow nanoparticle size distribution which minimizes inhomogeneous broadening of the spectrum and the presence of hydrogen atoms oscillating with the nanoparticle surfaces which enhances the number of scattered neutrons.
