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1.
Nat Commun ; 15(1): 3107, 2024 Apr 10.
Artigo em Inglês | MEDLINE | ID: mdl-38600083

RESUMO

The frequency scaling exponent of low-frequency excitations in microscopically small glasses, which do not allow for the existence of waves (phonons), has been in the focus of the recent literature. The density of states g(ω) of these modes obeys an ωs scaling, where the exponent s, ranging between 2 and 5, depends on the quenching protocol. The orgin of these findings remains controversal. Here we show, using heterogeneous-elasticity theory, that in a marginally-stable glass sample g(ω) follows a Debye-like scaling (s = 2), and the associated excitations (type-I) are of random-matrix type. Further, using a generalisation of the theory, we demonstrate that in more stable samples, other, (type-II) excitations prevail, which are non-irrotational oscillations, associated with local frozen-in stresses. The corresponding frequency scaling exponent s is governed by the statistics of small values of the stresses and, therefore, depends on the details of the interaction potential.

2.
Sci Rep ; 13(1): 21442, 2023 Dec 05.
Artigo em Inglês | MEDLINE | ID: mdl-38052816

RESUMO

Since decades, the concept of vibrational density of states in glasses has been mirrored in liquids by the instantaneous-normal-mode spectrum. In glasses instantaneous configurations are believed to be situated close to minima of the potential-energy hypersurface and all eigenvalues of the associated Hessian matrix are positive. In liquids this is no longer true, and modes corresponding to both positive and negative eigenvalues exist. The instantaneous-normal-mode spectrum has been numerically investigated in the past, and it has been demonstrated to bring important information on the liquid dynamics and transport properties. A systematic deeper theoretical understanding is now needed. Heterogeneous-elasticity theory has proven to be particularly successful in explaining many details of the low-frequency excitations in glasses, ranging from the thoroughly studied boson peak, to other anomalies related to the crossover between wave-like and random-matrix-like excitations. Here we present an extension of heterogeneous-elasticity theory to the liquid state, and show that the outcome of the theory agrees well to the results of extensive molecular-dynamics simulations of a model liquid at different temperatures. We find that the spectrum of eigenvalues [Formula: see text] has a sharp maximum close to (but not at) [Formula: see text], and decreases monotonically with [Formula: see text] on both its stable and unstable side. We show that the spectral shape strongly depends on temperature, being symmetric at high temperatures and becoming rather asymmetric at low temperatures, close to the dynamical critical temperature. Most importantly, we demonstrate that the theory naturally reproduces a surprising phenomenon, a zero-energy spectral singularity with a cusp-like character developing in the vibrational spectra upon cooling. This feature, known from a few previous numerical studies, has been generally overlooked in the past due to a misleading representation of the data. We provide a thorough analysis of this issue, based on both very accurate predictions of our theory, and computational studies of model liquid systems with extended size.

3.
Phys Rev E ; 106(3-2): 036601, 2022 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-36266813

RESUMO

We discuss a field-theoretical approach to liquids, solids, and glasses, published recently [Phys. Rev. E 105, 034108 (2022)10.1103/PhysRevE.105.034108], which aims to describe these materials in a common formalism. We argue that such a formalism contradicts the known hydrodynamic theory of classical liquids. In particular, the authors miss the important particle-number conservation law and the density fluctuations as a hydrodynamic slow variable. This results in an exotic mechanism of hydrodynamic sound instead of the standard hydrodynamic one due to combined particle-number and momentum conservation, a fact well documented in fluid-mechanics textbooks.

4.
Proc Natl Acad Sci U S A ; 119(8)2022 02 22.
Artigo em Inglês | MEDLINE | ID: mdl-35169078

RESUMO

We study the instantaneous normal mode (INM) spectrum of a simulated soft-sphere liquid at different equilibrium temperatures T We find that the spectrum of eigenvalues [Formula: see text] has a sharp maximum near (but not at) [Formula: see text] and decreases monotonically with [Formula: see text] on both the stable and unstable sides of the spectrum. The spectral shape strongly depends on temperature. It is rather asymmetric at low temperatures (close to the dynamical critical temperature) and becomes symmetric at high temperatures. To explain these findings we present a mean-field theory for [Formula: see text], which is based on a heterogeneous elasticity model, in which the local shear moduli exhibit spatial fluctuations, including negative values. We find good agreement between the simulation data and the model calculations, done with the help of the self-consistent Born approximation (SCBA), when we take the variance of the fluctuations to be proportional to the temperature T More importantly, we find an empirical correlation of the positions of the maxima of [Formula: see text] with the low-frequency exponent of the density of the vibrational modes of the glasses obtained by quenching to [Formula: see text] from the temperature T We discuss the present findings in connection to the liquid to glass transformation and its precursor phenomena.

5.
Phys Rev E ; 106(6-2): 066101, 2022 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-36671166

RESUMO

In a recent paper [Phys. Rev. E 104, 014103 (2021)10.1103/PhysRevE.104.014103] Baggioli and Zaccone formulate a theoretical description of the specific heat of liquids by using Debye's expression for the specific heat of solids and inserting a density of states which they claim to represent the instantaneous-normal-mode (INM) spectrum of a liquid. However, the quantum-mechanical procedure of Debye cannot be used for the relaxational excitations of a classical liquid. Furthermore, the authors' formula for the INM spectrum does not represent the known INM spectra of simple liquids, and the derivation of this formula from their model equation of motion is mathematically in error. These and a number of other inconsistencies render their work not very helpful for studying the specific heat of liquids.


Assuntos
Temperatura Alta , Movimento (Física)
6.
Sci Rep ; 11(1): 24454, 2021 Dec 27.
Artigo em Inglês | MEDLINE | ID: mdl-34961778

RESUMO

We report the effect of structural compaction on the statistics of elastic disorder in a silicate glass, using heterogeneous elasticity theory with the coherent potential approximation (HET-CPA) and a log-normal distribution of the spatial fluctuations of the shear modulus. The object of our study, a soda lime magnesia silicate glass, is compacted by hot-compression up to 2 GPa (corresponding to a permanent densification of ~ 5%). Using THz vibrational spectroscopic data and bulk mechanical properties as inputs, HET-CPA evaluates the degree of disorder in terms of the length-scale of elastic fluctuations and the non-affine part of the shear modulus. Permanent densification decreases the extent of non-affine elasticity, resulting in a more homogeneous distribution of strain energy, while also decreasing the correlation length of elastic heterogeneity. Complementary 29Si magic angle spinning NMR spectroscopic data provide a short-range rationale for the effect of compression on glass structure in terms of a narrowing of the Si-O-Si bond-angle and the Si-Si distance.

9.
Phys Rev Lett ; 120(6): 067401, 2018 Feb 09.
Artigo em Inglês | MEDLINE | ID: mdl-29481270

RESUMO

Anderson localization of light is traditionally described in analogy to electrons in a random potential. Within this description, the random potential depends on the wavelength of the incident light. For transverse Anderson localization, this leads to the prediction that the distribution of localization lengths-and, hence, its average-strongly depends on the wavelength. In an alternative description, in terms of a spatially fluctuating electric modulus, this is not the case. Here, we report on an experimentum crucis in order to investigate the validity of the two conflicting theories using optical samples exhibiting transverse Anderson localization. We do not find any dependence of the observed average localization radii on the light wavelength. We conclude that the modulus-type description is the correct one and not the potential-type one. We corroborate this by showing that in the derivation of the traditional potential-type theory, a term in the wave equation has been tacitly neglected. In our new modulus-type theory, the wave equation is exact. We check the consistency of the new theory with our data using the nonlinear sigma model. We comment on the consequences for the general case of three-dimensional disorder.

10.
Nat Commun ; 8: 14571, 2017 03 06.
Artigo em Inglês | MEDLINE | ID: mdl-28262763

RESUMO

Localized states trap waves propagating in a disordered potential and play a crucial role in Anderson localization, which is the absence of diffusion due to disorder. Some localized states are barely coupled with neighbours because of differences in wavelength or small spatial overlap, thus preventing energy leakage to the surroundings. This is the same degree of isolation found in the homogeneous core of a single-mode optical fibre. Here we show that localized states of a disordered optical fibre are single mode: the transmission channels possess a high degree of resilience to perturbation and invariance with respect to the launch conditions. Our experimental approach allows identification and characterization of the single-mode transmission channels in a disordered matrix, demonstrating low losses and densely packed single modes. These disordered and wavelength-sensitive channels may be exploited to de-multiplex different colours at different locations.

11.
Phys Rev Lett ; 115(24): 240602, 2015 Dec 11.
Artigo em Inglês | MEDLINE | ID: mdl-26705618

RESUMO

By event-driven molecular dynamics simulations we investigate magnetotransport in a two-dimensional model with randomly distributed scatterers close to the field-induced localization transition. This transition is generated by percolating skipping orbits along the edges of obstacle clusters. The dynamic exponents differ significantly from those of the conventional transport problem on percolating systems, thus establishing a new dynamic universality class. This difference is tentatively attributed to a weak-link scenario, which emerges naturally due to barely overlapping edge trajectories. We make predictions for the frequency-dependent conductivity and discuss implications for active colloidal circle swimmers in a hetegogeneous environment.

12.
Phys Rev Lett ; 115(1): 015901, 2015 Jul 03.
Artigo em Inglês | MEDLINE | ID: mdl-26182108

RESUMO

We present a heterogeneous version of Maxwell's theory of viscoelasticity based on the assumption of spatially fluctuating local viscoelastic coefficients. The model is solved in coherent-potential approximation. The theory predicts an Arrhenius-type temperature dependence of the viscosity in the vanishing-frequency limit, independent of the distribution of the activation energies. It is shown that this activation energy is generally different from that of a diffusing particle with the same barrier-height distribution, which explains the violation of the Stokes-Einstein relation observed frequently in glasses. At finite but low frequencies, the theory describes low-temperature asymmetric alpha relaxation. As examples, we report the good agreement obtained for selected inorganic, metallic, and organic glasses. At high frequencies, the theory reduces to heterogeneous elasticity theory, which explains the occurrence of the boson peak and related vibrational anomalies.

13.
Sci Rep ; 3: 1407, 2013.
Artigo em Inglês | MEDLINE | ID: mdl-23470597

RESUMO

The local elasticity of glasses is known to be inhomogeneous on a microscopic scale compared to that of crystalline materials. Their vibrational spectrum strongly deviates from that expected from Debye's elasticity theory: The density of states deviates from Debye's law, the sound velocity shows a negative dispersion in the boson-peak frequency regime and there is a strong increase of the sound attenuation near the boson-peak frequency. By comparing a mean-field theory of shear-elastic heterogeneity with a large-scale simulation of a soft-sphere glass we demonstrate that the observed anomalies in glasses are caused by elastic heterogeneity. By observing that the macroscopic bulk modulus is frequency independent we show that the boson-peak-related vibrational anomalies are predominantly due to the spatially fluctuating microscopic shear stresses. It is demonstrated that the boson-peak arises from the steep increase of the sound attenuation at a frequency which marks the transition from wave-like excitations to disorder-dominated ones.

14.
Phys Rev Lett ; 100(13): 137402, 2008 Apr 04.
Artigo em Inglês | MEDLINE | ID: mdl-18517995

RESUMO

We present a theory of low-frequency Raman scattering in glasses, based on the concept that light couples to the elastic strains via spatially fluctuating elasto-optic (Pockels) constants. We show that the Raman intensity is not proportional to the vibrational density of states (as was widely believed), but to a convolution of Pockels constant correlation functions with the dynamic strain susceptibilities of the glass. Using the dynamic susceptibilities of a system with fluctuating elastic constants we are able for the first time to describe the Raman intensity and the anomalous vibration spectrum of a glass on the same footing. Good agreement between the theory and experiment for the Raman spectrum, the density of states, and the specific heat is demonstrated at the example of glassy As(2)S(3).

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