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Register a new userMicroscopic dynamics of supercooled liquids from first principles
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Glasses are solid materials whose constituent atoms are arranged in a disordered manner. The transition from a liquid to a glass remains one of the most poorly understood phenomena in condensed matter physics, and still no fully microscopic theory exists that can describe the dynamics of supercooled liquids in a quantitative manner over all relevant time scales. Here we present such a theoretical framework that yields near-quantitative accuracy for the time-dependent correlation functions of a supercooled system over a broad density range. Our approach requires only simple static structural information as input and is based entirely based on first principles. Owing to this first-principles nature, the framework offers a unique platform to study the relation between structure and dynamics in glass-forming matter, and paves the way towards a systematically correctable and ultimately fully quantitative theory of microscopic glassy dynamics.
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It was recently demonstrated that a simple Monte Carlo (MC) algorithm involving the swap of particle pairs dramatically accelerates the equilibrium sampling of simulated supercooled liquids. We propose two numerical schemes integrating the efficiency of particle swaps into equilibrium molecular dynamics (MD) simulations. We first develop a hybrid MD/MC scheme combining molecular dynamics with the original swap Monte Carlo. We implement this hybrid method in LAMMPS, a software package employed by a large community of users. Secondly, we define a continuous time version of the swap algorithm where both the positions and diameters of the particles evolve via Hamiltons equations of motion. For both algorithms, we discuss in detail various technical issues as well as the optimisation of simulation parameters. We compare the numerical efficiency of all available swap algorithms and discuss their relative merits.
We compare the spatial correlations of bond-breaking events and bond-orientational relaxation in a model two-dimensional liquid undergoing Newtonian dynamics. We find that the relaxation time of the bond-breaking correlation function is much longer than the relaxation time of the bond-orientational correlation function and self-intermediate scattering function. However, the relaxation time of the bond-orientational correlation function increases faster with decreasing temperature than the relaxation time of the bond-breaking correlation function and the self-intermediate scattering function. Moreover, the dynamic correlation length that characterizes the size of correlated bond-orientational relaxation grows faster with decreasing temperature than the dynamic correlation length that characterizes the size of correlated bond-breaking events. We also examine the ensemble-dependent and ensemble-independent dynamic susceptibilities for both bond-breaking correlations and bond-orientational correlations. We find that for both correlations, the ensemble-dependent and ensemble-independent susceptibilities exhibit a maximum at nearly the same time, and this maximum occurs at a time slightly shorter than the peak position of the dynamic correlation length.
Freezing is a fundamental physical phenomenon that has been studied over many decades; yet the role played by surfaces in determining nucleation has remained elusive. Here we report direct computational evidence of surface induced nucleation in supercooled systems with a negative slope of their melting line (dP/dT < 0). This unexpected result is related to the density decrease occurring upon crystallization, and to surface tension facilitating the initial nucleus formation. Our findings support the hypothesis of surface induced crystallization of ice in the atmosphere, and provide insight, at the atomistic level, into nucleation mechanisms of widely used semiconductors.
A theoretical treatment of deeply supercooled liquids is difficult because their properties emerge from spatial inhomogeneities that are self-induced, transient, and nanoscopic. I use computer simulations to analyse self-induced static and dynamic heterogeneity in equilibrium systems approaching the experimental glass transition. I characterise the broad sample-to-sample fluctuations of salient dynamic and thermodynamic properties in elementary mesoscopic systems. Findings regarding local lifetimes and distributions of dynamic heterogeneity are in excellent agreement with recent single molecule studies. Surprisingly broad thermodynamic fluctuations are also found, which correlate well with dynamics fluctuations, thus providing a local test of the thermodynamic origin of slow dynamics.
The mode-coupling theory of the glass transition treats the dynamics of supercooled liquids in terms of two-point density correlation functions. Here we consider a generalized, hierarchical formulation of schematic mode-coupling equations in which the full basis of multipoint density correlations is taken into account. By varying the parameters that control the effective contributions of higher-order correlations, we show that infinite hierarchies can give rise to both sharp and avoided glass transitions. Moreover, small changes in the form of the coefficients result in different scaling behaviors of the structural relaxation time, providing a means to tune the fragility in glass-forming materials. This demonstrates that the infinite-order construct of generalized mode-coupling theory constitutes a powerful and unifying framework for kinetic theories of the glass transition.
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