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Sound attenuation in finite-temperature stable glasses

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 Added by Elijah Flenner
 Publication date 2020
  fields Physics
and research's language is English




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The temperature dependence of the thermal conductivity of amorphous solids is markedly different from that of their crystalline counterparts, but exhibits universal behaviour. Sound attenuation is believed to be related to this universal behaviour. Recent computer simulations demonstrated that in the harmonic approximation sound attenuation $Gamma$ obeys quartic, Rayleigh scattering scaling for small wavevectors $k$ and quadratic scaling for wavevectors above the Ioffe-Regel limit. However, simulations and experiments do not provide a clear picture of what to expect at finite temperatures where anharmonic effects become relevant. Here we study sound attenuation at finite temperatures for model glasses of various stability, from unstable glasses that exhibit rapid aging to glasses whose stability is equal to those created in laboratory experiments. We find several scaling laws depending on the temperature and stability of the glass. First, we find the large wavevector quadratic scaling to be unchanged at all temperatures. Second, we find that at small wavectors $Gamma sim k^{1.5}$ for an aging glass, but $Gamma sim k^2$ when the glass does not age on the timescale of the calculation. For our most stable glass, we find that $Gamma sim k^2$ at small wavevectors, then a crossover to Rayleigh scattering scaling $Gamma sim k^4$, followed by another crossover to the quadratic scaling at large wavevectors. Our computational observation of this quadratic behavior reconciles simulation, theory and experiment, and will advance the understanding of the temperature dependence of thermal conductivity of glasses.

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The attenuation of long-wavelength phonons (waves) by glassy disorder plays a central role in various glass anomalies, yet it is neither fully characterized, nor fully understood. Of particular importance is the scaling of the attenuation rate $Gamma(k)$ with small wavenumbers $k!to!0$ in the thermodynamic limit of macroscopic glasses. Here we use a combination of theory and extensive computer simulations to show that the macroscopic low-frequency behavior emerges at intermediate frequencies in finite-size glasses, above a recently identified crossover wavenumber $k_dagger$, where phonons are no longer quantized into bands. For $k!<!k_dagger$, finite-size effects dominate $Gamma(k)$, which is quantitatively described by a theory of disordered phonon bands. For $k!>!k_dagger$, we find that $Gamma(k)$ is affected by the number of quasilocalized nonphononic excitations, a generic signature of glasses that feature a universal density of states. In particular, we show that in a frequency range in which this number is small, $Gamma(k)$ follows a Rayleigh scattering scaling $sim!k^{d+1}$ ($d$ is the spatial dimension), and that in a frequency range in which this number is sufficiently large, the recently observed generalized-Rayleigh scaling of the form $sim!k^{d+1}log!{(k_0/k)}$ emerges ($k_0!>k_dagger$ is a characteristic wavenumber). Our results suggest that macroscopic glasses --- and, in particular, glasses generated by conventional laboratory quenches that are known to strongly suppress quasilocalized nonphononic excitations --- exhibit Rayleigh scaling at the lowest wavenumbers $k$ and a crossover to generalized-Rayleigh scaling at higher $k$. Some supporting experimental evidence from recent literature is presented.
Three classes of harmonic disorder systems (Lennard-Jones like glasses, percolators above threshold, and spring disordered lattices) have been numerically investigated in order to clarify the effect of different types of disorder on the mechanism of high frequency sound attenuation. We introduce the concept of frustration in structural glasses as a measure of the internal stress, and find a strong correlation between the degree of frustration and the exponent alpha that characterizes the momentum dependence of the sound attenuation $Gamma(Q)$$simeq$$Q^alpha$. In particular, alpha decreases from about d+1 in low-frustration systems (where d is the spectral dimension), to about 2 for high frustration systems like the realistic glasses examined.
81 - U. Buchenau 2020
The paper presents a description of the sound wave absorption in glasses, from the lowest temperatures up to the glass transition, in terms of two compatible phenomenological models. Resonant tunneling, the rise of the relaxational tunneling to the tunneling plateau and the crossover to classical relaxation are universal features of glasses and are well described by the extension of the tunneling model to include soft vibrations and low barrier relaxations, the soft potential model. Its further extension to non-universal features at higher temperatures is the very flexible Gilroy-Phillips model, which allows to determine the barrier density of the energy landscape of the specific glass from the frequency and temperature dependence of the sound wave absorption in the classical relaxation domain. To apply it properly at elevated temperatures, one needs its formulation in terms of the shear compliance. As one approaches the glass transition, universality sets in again with an exponential rise of the barrier density reflecting the frozen fast Kohlrausch t^beta-tail (in time t, with beta close to 1/2) of the viscous flow at the glass temperature. The validity of the scheme is checked for literature data of several glasses and polymers with and without secondary relaxation peaks. The frozen Kohlrausch tail of the mechanical relaxation shows no indication of the strongly temperature-dependent excess wing observed in dielectric data of molecular glasses with hydrogen bonds. Instead, the mechanical relaxation data indicate an energy landscape describable with a frozen temperature-independent barrier density for any glass.
The precipitation of a glass forming solute from solution is modelled using a lattice model previously introduced to study dissolution kinetics of amorphous materials. The model includes the enhancement of kinetics at the surface of a glass in contact with a plasticizing solvent. We demonstrate that precipitation can produce a glass substantially more stable than that produced by very long time annealing of the bulk glass former. The energy of these ultra-stable amorphous precipitates is found to be dominated by residual solvent rather than high energy glass configurations.
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