We investigate acoustic propagation in amorphous solids by constructing a projection formalism based on separating atomic vibrations into two, "phonon" (P) and "non-phonon" (NP), subspaces corresponding to large and small wavelengths. For a pairwise interaction model, we show the existence of a "natural" separation lengthscale, determined by structural disorder, for which the isolated P subspace presents the acoustic properties of a nearly homogenous (Debye-like) elastic continuum, while the NP one encapsulates all small scale non-affinity effects. The NP eigenstates then play the role of dynamical scatterers for the phonons. However, at variance with a conjecture of defect theories, their spectra present a finite low frequency gap, which turns out to lie around the Boson peak frequency, and only a small fraction of them are highly localized. We then show that small scale disorder effects can be rigorously reduced to the existence, in the Navier-like wave equation of the continuum, of a generalized elasticity tensor, which is not only retarded, since scatterers are dynamical, but also non-local. The full neglect of both retardation and non-locality suffices to account for most of the corrections to Born macroscopic moduli. However, these two features are responsible for sound speed dispersion and have quite a significant effect on the magnitude of sound attenuation. Although it remains open how they impact the asymptotic, large wavelength scaling of sound damping, our findings rule out the possibility of representing an amorphous solid by an inhomogeneous elastic continuum with the standard (i.e., local and static) elastic moduli.
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J Chem Phys
October 2020
NAVIER, UMR 8205, École des Ponts ParisTech, IFSTTAR, CNRS, UPE, Champs-sur-Marne, France.
We investigate acoustic propagation in amorphous solids by constructing a projection formalism based on separating atomic vibrations into two, "phonon" (P) and "non-phonon" (NP), subspaces corresponding to large and small wavelengths. For a pairwise interaction model, we show the existence of a "natural" separation lengthscale, determined by structural disorder, for which the isolated P subspace presents the acoustic properties of a nearly homogenous (Debye-like) elastic continuum, while the NP one encapsulates all small scale non-affinity effects. The NP eigenstates then play the role of dynamical scatterers for the phonons.
View Article and Find Full Text PDFJ Chem Phys
April 2018
Dipartimento di Fisica e Astronomia, Università degli Studi di Padova, Via Marzolo 8, 35131 Padova, Italy.
Dispersion forces play a major role in graphene, largely influencing adhesion of adsorbate moieties and stabilization of functional multilayered structures. However, the reliable prediction of dispersion interactions on graphene up to the relevant ∼10 nm scale is an extremely challenging task: in fact, electromagnetic retardation effects and the highly non-local character of π electrons can imply sizeable qualitative variations of the interaction with respect to known pairwise approaches. Here we address both issues, determining the finite-temperature van der Waals (vdW)-Casimir interaction for point-like and extended adsorbates on graphene, explicitly accounting for the non-local dielectric permittivity.
View Article and Find Full Text PDFChem Soc Rev
September 2008
Instituto de Optica-CSIC, Serrano 121, 28006 Madrid, Spain.
This tutorial review presents an overview of theoretical methods for predicting and understanding the optical response of gold nanoparticles. A critical comparison is provided, assisting the reader in making a rational choice for each particular problem, while analytical models provide insights into the effects of retardation in large particles and non-locality in small particles. Far- and near-field spectra are discussed, and the relevance of the latter in surface-enhanced Raman spectroscopy and electron energy-loss spectroscopy is emphasized.
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