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Register a new userDisentangling interatomic repulsion and anharmonicity in the viscosity and fragility of glasses
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Within the shoving model of the glass transition, the relaxation time and the viscosity are related to the local cage rigidity. This approach can be extended down to the atomic-level in terms of the interatomic interaction, or potential of mean-force. We applied this approach to both real metallic glass-formers and model Lennard-Jones glasses. The main outcome of this analysis is that in metallic glasses the thermal expansion contribution is mostly independent of composition and is uncorrelated with the interatomic repulsion: as a consequence, the fragility increases upon increasing the interatomic repulsion steepness. In the Lennard-Jones glasses, the scenario is opposite: thermal expansion and interatomic repulsion contributions are strongly correlated, and the fragility decreases upon increasing the repulsion steepness. This framework allows one to tell apart systems where soft atoms make strong glasses from those where, instead, soft atoms make fragile glasses. Hence, it opens up the way for the rational, atomistic tuning of the fragility and viscosity of widely different glass-forming materials all the way from strong to fragile.
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We show that a {em vibrational instability} of the spectrum of weakly interacting quasi-local harmonic modes creates the maximum in the inelastic scattering intensity in glasses, the Boson peak. The instability, limited by anharmonicity, causes a complete reconstruction of the vibrational density of states (DOS) below some frequency $omega_c$, proportional to the strength of interaction. The DOS of the new {em harmonic modes} is independent of the actual value of the anharmonicity. It is a universal function of frequency depending on a single parameter -- the Boson peak frequency, $omega_b$ which is a function of interaction strength. The excess of the DOS over the Debye value is $proptoomega^4$ at low frequencies and linear in $omega$ in the interval $omega_b ll omega ll omega_c$. Our results are in an excellent agreement with recent experimental studies.
A recently published analytical model, describing and predicting elasticity, viscosity, and fragility of metallic melts, is applied for the analysis of about 30 nonmetallic glassy systems, ranging from oxide network glasses to alcohols, low-molecular-weight liquids, polymers, plastic crystals, and even ionic glass formers. The model is based on the power-law exponent lambda representing the steepness parameter of the repulsive part of the inter-atomic or -molecular potential and the thermal-expansion parameter alpha_T determined by the attractive anharmonic part of the effective interaction. It allows fitting the typical super-Arrhenius temperature variation of the viscosity or dielectric relaxation time for various classes of glass-forming matter, over many decades. We discuss the relation of the model parameters found for all these different glass-forming systems to the fragility parameter m and detect a correlation of lambda and m for the non-metallic glass formers, in accord with the model predictions. Within the framework of this model, thus the fragility of glass formers can be traced back to microscopic model parameters characterizing the intermolecular interactions.
We report experiments on hard sphere colloidal glasses that reveal a type of shear banding hitherto unobserved in soft glasses. We present a scenario that relates this to an instability arising from shear-concentration coupling, a mechanism previously thought unimportant in this class of materials. Below a characteristic shear rate $dotgamma_c$ we observe increasingly non-linear velocity profiles and strongly localized flows. We attribute this trend to very slight concentration gradients (likely to evade direct detection) arising in the unstable flow regime. A simple model accounts for both the observed increase of $dotgamma_c$ with concentration, and the fluctuations observed in the flow.
The evolution of porous structure, potential energy and local density in binary glasses under oscillatory shear deformation is investigated using molecular dynamics simulations. The porous glasses were initially prepared via a rapid thermal quench from the liquid state across the glass transition and allowed to phase separate and solidify at constant volume, thus producing an extended porous network in an amorphous solid. We find that under periodic shear, the potential energy decreases over consecutive cycles due to gradual rearrangement of the glassy material, and the minimum of the potential energy after thousands of shear cycles is lower at larger strain amplitudes. Moreover, with increasing cycle number, the pore size distributions become more skewed toward larger length scales where a distinct peak is developed and the peak intensity is enhanced at larger strain amplitudes. The numerical analysis of the local density distribution functions demonstrates that cyclic loading leads to formation of higher density solid domains and homogenization of the glass phase with reduced density.
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.
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