0000000000200125
AUTHOR
Daniel B. Murray
Continuum elastic sphere vibrations as a model for low-lying optical modes in icosahedral quasicrystals
The nearly dispersionless, so-called "optical" vibrational modes observed by inelastic neutron scattering from icosahedral Al-Pd-Mn and Zn-Mg-Y quasicrystals are found to correspond well to modes of a continuum elastic sphere that has the same diameter as the corresponding icosahedral basic units of the quasicrystal. When the sphere is considered as free, most of the experimentally found modes can be accounted for, in both systems. Taking into account the mechanical connection between the clusters and the remainder of the quasicrystal allows a complete assignment of all optical modes in the case of Al-Pd-Mn. This approach provides support to the relevance of clusters in the vibrational prop…
Millimeter wave absorption by confined acoustic modes in CdSe/CdTe core-shell quantum dots
International audience; Taking advantage of the specific core-shell charge separation structure in the CdSe/CdTe core-shell Type-II quantum dots (QDs), we experimentally observed the resonant-enhanced dipolar interaction between millimeter-wave (MMW) photons and their corresponding (l = 1) confined acoustic phonons. With proper choice of size, the absorption band can be tuned to desired frequency of MMW imaging. Exploiting this characteristic absorption, in a fiber-scanned MMW imaging system, we demonstrated the feasibility of CdSe/CdTe QDs as the contrast agents of MMW imaging.
High precision numerical estimates of acoustic phonon frequencies of nonspherical nanoparticles
We introduce an adapted method for calculating the acoustic vibrational frequencies of arbitrarily shaped nanoparticles to high precision. Molecular dynamics simulation results are tested against exact solutions for a free sphere, a hollow sphere and a spheroid. This permits theoretical predictions of the frequencies of peaks in low frequency Raman spectra. Our results demonstrate that vibrational frequencies can be calculated for a wide range of low frequency modes with accuracies on the order of a tenth of a percent.
Far infrared absorption by acoustic phonons in titanium dioxide nanopowders
We report spectral features of far infrared electromagnetic radiation absorption in anatase TiO2 nanopowders which we attribute to absorption by acoustic phonon modes of nanoparticles. The frequency of peak excess absorption above the background level corresponds to the predicted frequency of the dipolar acoustic phonon from continuum elastic theory. The intensity of the absorption cannot be accounted for in a continuum elastic dielectric description of the nanoparticle material. Quantum mechanical scale dependent effects must be considered. The absorption cross section is estimated from a simple mechanical phenomenological model. The results are in plausible agreement with the absorption b…
Vibrations of weakly coupled nanoparticles
The vibrations of a coupled pair of isotropic silver spheres are investigated and compared with the vibrations of the single isolated spheres. Situations of both strong coupling and also weak coupling are investigated using continuum elasticity and perturbation theory. The numerical calculation of the eigenmodes of such dimers is augmented with a symmetry analysis. This checks the convergence and applicability of the numerical method and shows how the eigenmodes of the dimer are constructed from those of the isolated spheres. The frequencies of the lowest frequency vibrations of such dimers are shown to be very sensitive to the strength of the coupling between the spheres. Some of these mod…
Long Lived Acoustic Vibrational Modes of an Embedded Nanoparticle
Classical continuum elastic calculations show that the acoustic vibrational modes of an embedded nanoparticle can be lightly damped even when the longitudinal plane wave acoustic impedances $Z_o=\rho v_L$ of the nanoparticle and the matrix are the same. It is not necessary for the matrix to be less dense or softer than the nanoparticle in order to have long lived vibrational modes. Continuum boundary conditions do not always accurately reflect the microscropic nature of the interface between nanoparticle and matrix, and a multi-layer model of the interface reveals the possibility of additional reduction of mode damping.
Surface plasmons and vibrations of self-assembled silver nanocolumns
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Inelastic neutron scattering due to acoustic vibrations confined in nanoparticles: theory and experiment
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 enhan…
Simple model for the vibrations of embedded elastically cubic nanocrystals
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 embedded 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.
Damping by Bulk and Shear Viscosity of Confined Acoustic Phonons for Nanostructures in Aqueous Solution
International audience; A nanoparticle in aqueous solution is modeled as a homogeneous elastic isotropic continuum sphere in contact with an infinite viscous compressible Newtonian fluid. The frequencies and damping of the confined vibrational modes of the sphere are calculated for the material parameters of a CdSe nanoparticle in water and a poly(methyl methacrylate) nanosphere in water. Although the effects of viscosity are found to be negligible for macroscopic objects, for nanoscale objects, both the frequency and damping of the vibrational modes are significantly affected by the viscosity of the liquid. Furthermore, both shear viscosity and bulk viscosity play an important role. A mode…
Vibrations of free and embedded anisotropic elastic spheres:Application to low-frequency Raman scattering of silicon nanoparticles in silica
Vibrational mode frequencies and damping are calculated for an elastic sphere embedded in an infinite, homogeneous, isotropic elastic medium. Anisotropic elasticity of the sphere significantly shifts the frequencies in comparison to simplified calculations that assume isotropy. New low-frequency Raman light scattering data are presented for silicon spheres grown in a ${\mathrm{SiO}}_{2}$ glass matrix. Principal features of the Raman spectrum are not correctly described by a simple model of the nanoparticle as a free, isotropic sphere, but require both matrix effects and the anisotropy of the silicon to be taken into account. Libration, not vibration, is the dominant mechanism.
Surface enhanced Raman scattering of silver sensitized cobalt nanoparticles in metal–dielectric nanocomposites
We report the preparation of a new type of nanocomposite containing cobalt and silver nanoparticles organized in parallel layers with a well controlled separation. This arrangement allows the observation of an enhanced low-frequency Raman signal at the vibration frequency of cobalt nanoparticles excited through the surface plasmons of silver nanoparticles. Numerical simulations of the electric field confirm the emergence of hot spots when the separation between silver and cobalt nanoparticles is small enough. © IOP Publishing Ltd.
Acoustic vibrations of anisotropic nanoparticles
Acoustic vibrations of nanoparticles made of materials with anisotropic elasticity and nanoparticles with non-spherical shapes are theoretically investigated using a homogeneous continuum model. Cubic, hexagonal and tetragonal symmetries of the elasticity are discussed, as are spheroidal, cuboctahedral and truncated cuboctahedral shapes. Tools are described to classify the different vibrations and for example help identify the modes having a significant low-frequency Raman scattering cross-section. Continuous evolutions of the modes starting from those of an isotropic sphere coupled with the determination of the irreducible representation of the branches permit some qualitative statements t…
Quasi-free nanoparticle vibrations in a highly-compressed ZrO2 nanopowder
Several-nanometer-size mechanical oscillators, or nanoresonators, may complement electronic and optical technologies in future terahertz devices, but they can be useful only if they can be made to ...
Phonons in an inhomogeneous continuum: Vibrations of an embedded nanoparticle
The spectrum of acoustic vibrational modes of an inhomogeneous elastic continuum are analyzed with application to a spherical nanoparticle embedded in an infinite glass block. The relationship of these modes to the discrete vibrational spectrum of a free sphere is studied. The vibrational modes of a sphere with a fixed surface are relevant in some situations. Comparisons are also made to calculations of mode frequency and damping based on complex valued frequency.
Acoustic vibrations of embedded spherical nanoparticles
Abstract A solid-matrix-embedded spherical nanoparticle has acoustic vibrational frequencies which are shifted and damped relative to modes of a free sphere. Not only the longitudinal plane wave acoustic impedances, but also the Poisson ratios of nanoparticle and matrix are important in determining the Q-factor of the “breathing” mode, for which frequencies and Q-factors with different material combinations are presented. High matrix sound speed (e.g. silica, titania, alumina, diamond) increases Q.
THz nanocrystal acoustic vibrations from ZrO2 3D supercrystals
International audience; We report sharp low-frequency Raman spectral features of supercrystals synthesized via the "benzyl alcohol route" and consisting of either yttrium-stabilized or pure zirconia (ZrO2) nanocrystals. In situ formed benzoate species control the nanocrystal growth and act as organic glue leading to the assembly of the nanocrystals in highly ordered 3D supercrystals. We attribute some Raman peaks to THz acoustic vibrations of individual nanocrystals which are only weakly coupled due to the strong acoustic mismatch between the capping ligands and the nanocrystals. Peak positions are consistent with nanocrystal sizes estimated from transmission electron microscopy and X-ray p…
Damping by bulk and shear viscosity for confined acoustic phonons of a spherical virus in water
International audience; A sphere-like virus in water is modeled as a homogeneous isotropic elastic continuum sphere in contact with an infinite viscous compressible Newtonian fluid. The frequencies and damping of the confined vibrational modes of the sphere are calculated for the material parameters of a virus in water. While the effects of viscosity are found to be negligible for a virus-like sphere of macroscopic size, for nanoscale viruses both the frequency and damping of the vibrational modes are significantly affected by the viscosity of the water. Furthermore, both shear viscosity and bulk viscosity play an important role.
Longitudinal versus transverse spheroidal vibrational modes of an elastic sphere
Analysis of the spheroidal modes of vibration of a free elastic sphere show that they can be qualitatively grouped into two categories: primarily longitudinal and primarily transverse. This is not a sharp distinction. However, there is a relatively stark contrast between the two kinds of modes. Primarily transverse modes have a small divergence and have frequencies that are almost functionally independent of the longitudinal speed of sound. Analysis of inelastic light scattering intensity from confined acoustic phonons in nanoparticles requires an understanding of this qualitative distinction between different spheroidal modes. In addition, some common misconceptions about spheroidal modes …