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Register a new userIs the Fragility of a Liquid Embedded in the Properties of its Glass?
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When a liquid is cooled below its melting temperature it usually crystallizes. However, if the quenching rate is fast enough, it is possible that the system remains in a disordered state, progressively losing its fluidity upon further cooling. When the time needed for the rearrangement of the local atomic structure reaches approximately 100 seconds, the system becomes solid for any practical purpose, and this defines the glass transition temperature $T_g$. Approaching this transition from the liquid side, different systems show qualitatively different temperature dependencies of the viscosity, and, accordingly, they have been classified introducing the concept of fragility. We report experimental observations that relate the microscopic properties of the {it glassy phase} to the fragility. We find that the vibrational properties of the glass {it well below} $T_g$ are correlated with the fragility value. Consequently, we extend the fragility concept to the glassy state and indicate how to determine the fragility uniquely from glass properties well below $T_g$.
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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.
Using molecular dynamics simulations we investigate the dependence of the structural and vibrational properties of the surfaces of sodo-silicate glasses on the sodium content as well as the nature of the surface. Two types of glass surfaces are considered: A melt-formed surface (MS) in which a liquid with a free surface has been cooled down into the glass phase and a fracture surface (FS) obtained by tensile loading of a glass sample. We find that the MS is more abundant in Na and non-bridging oxygen atoms than the FS and the bulk glass, whereas the FS has higher concentration of structural defects such as two-membered rings and under-coordinated Si than the MS. We associate these structural differences to the production histories of the glasses and the mobility of the Na ions. It is also found that for Na-poor systems the fluctuations in composition and local atomic charge density decay with a power-law as a function of distance from the surface while Na-rich systems show an exponential decay with a typical decay length of $approx2.3$~AA. The vibrational density of states shows that the presence of the surfaces leads to a decrease of the characteristic frequencies in the system. The two-membered rings give rise to a pronounce band at $approx880$~cm$^{-1}$ which is in good agreement experimental observations.
If quenched fast enough, a liquid is able to avoid crystallization and will remain in a metastable supercooled state down to the glass transition, with an important increase in viscosity upon further cooling. There are important differences in the way liquids relax as they approach the glass transition, rapid or slow variation in dynamic quantities under moderate temperature changes, and a simple means to quantify such variations is provided by the concept of fragility. Here, we report molecular dynamics simulations of a typical network-forming glass, Ge-Se, and find that the relaxation behaviour of the supercooled liquid is strongly correlated to the variation of rigidity with temperature and the spatial distribution of the corresponding topological constraints which, ultimately connect to fragility minima. This permits extending the fragility concept to aspects of topology/rigidity, and to the degree of homogeneity of the atomic-sale interactions for a variety of structural glasses.
Effects of temperature changes on the nonequilibrium spin-glass dynamics of a strongly interacting ferromagnetic nanoparticle system (superspin glass) are studied. In contrary to atomic spin glasses, strong cooling rate effects are observed, and no evidence for temperature-chaos is found. The flip time of a magnetic moment is much longer than that of an atomic spin and hence much shorter time scales are probed within the experimental time window for a superspin glass than for an atomic spin glass. Within a real space picture the cumulative aging observed for the superspin glass can be explained considering that all investigated length scales are shorter than the temperature-chaos overlap length. The transient relaxation, observed in experiments after temperature changes, can be understood as the adjustment of thermally active droplets, which is mutatis mutandis the Kovacs effect observed in most glassy systems.
We show in numerical simulations that a system of two coupled replicas of a binary mixture of hard spheres undergoes a phase transition in equilibrium at a density slightly smaller than the glass transition density for an unreplicated system. This result is in agreement with the theories that predict that such a transition is a precursor of the standard ideal glass transition. The critical properties are compatible with those of an Ising system. The relations of this approach to the conventional approach based on configurational entropy are briefly discussed.
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