Understanding the glassy dynamics from melting temperatures in binary glass-forming liquids.

It is natural to expect that small particles in binary mixtures move faster than large ones. However, in binary glass-forming liquids with soft-core particle interactions, we observe the counterintuitive dynamic reversal between large and small particles along with the increase of pressure by performing molecular dynamics simulations. The structural relaxation (dynamic heterogeneity) of small particles is faster (weaker) than large ones at low pressures, but becomes slower (stronger) above a crossover pressure. In contrast, this dynamic reversal never happens in glass-forming liquids with hard-core interactions. We find that the difference of the effective melting temperatures felt by large and small particles can be used to understand the dynamic reversal. In binary mixtures, we derive effective melting temperatures of large and small particles simply from the conversion of units and find that particles with a higher effective melting temperature usually undergo a slower and more heterogeneous relaxation. The presence (absence) of the dynamic reversal in soft-core (hard-core) systems is simply due to the non-monotonic (monotonic) behavior of the melting temperature as a function of pressure. Interestingly, by manipulating the relative softness between large and small particles, we obtain a special case of soft-core systems, in which large particles always have higher effective melting temperatures than small ones. As a result, the dynamic reversal is totally eliminated. Our work provides another piece of evidence of the underlying connections between the properties of non-equilibrium glass-formers and equilibrium crystal-formers.

Density of states below the first sound mode in 3D glasses.

Glasses feature universally low-frequency excess vibrational modes beyond Debye prediction, which could help rationalize, e.g., the glasses' unusual temperature dependence of thermal properties compared to crystalline solids. The way the density of states of these low-frequency excess modes D(ω) depends on the frequency ω has been debated for decades. Recent simulation studies of 3D glasses suggest that D(ω) scales universally with ω4 in a low-frequency regime below the first sound mode. However, no simulation study has ever probed as low frequencies as possible to test directly whether this quartic law could work all the way to extremely low frequencies. Here, we calculated D(ω) below the first sound mode in 3D glasses over a wide range of frequencies. We find D(ω) scales with ωß with ß < 4 at very low frequencies examined, while the ω4 law works only in a limited intermediate-frequency regime in some glasses. Moreover, our further analysis suggests our observation does not depend on glass models or glass stabilities examined. The ω4 law of D(ω) below the first sound mode is dominant in current simulation studies of 3D glasses, and our direct observation of the breakdown of the quartic law at very low frequencies thus leaves an open but important question that may attract more future numerical and theoretical studies.

Unifying fluctuation-dissipation temperatures of slow-evolving nonequilibrium systems from the perspective of inherent structures.

For nonequilibrium systems, how to define temperature is one of the key and difficult issues to solve. Although effective temperatures have been proposed and studied to this end, it still remains elusive what they actually are. Here, we focus on the fluctuation-dissipation temperatures and report that such effective temperatures of slow-evolving systems represent characteristic temperatures of their equilibrium counterparts. By calculating the fluctuation-dissipation relation of inherent structures, we obtain a temperature-like quantity T IS For monocomponent crystal-formers, T IS agrees well with the crystallization temperature T c, while it matches with the onset temperature T on for glass-formers. It also agrees with effective temperatures of typical nonequilibrium systems, such as aging glasses, quasi-static shear flows, and quasi-static self-propelled flows. From the unique perspective of inherent structures, our study reveals the nature of effective temperatures and the underlying connections between nonequilibrium and equilibrium systems and confirms the equivalence between T on and T c.

Signatures of continuous hexatic-liquid transition in two-dimensional melting.

Recent studies have shown that the melting of two-dimensional crystals can be either continuous or discontinuous, relying on multiple parameters such as particle stiffness, density, and particle size dispersity. However, what determines the continuity or discontinuity of the two-dimensional melting remains elusive. Here we study the two-dimensional melting of binary mixtures of soft-core particles. The two particle species are different in either particle size or particle stiffness. Starting with the mono-component systems which exhibit discontinuous hexatic-liquid transition, we gradually increase the particle size or stiffness dispersity and find that the hexatic-liquid coexistent region shrinks and eventually vanishes above a critical dispersity. Therefore, the growth of disorder caused by the particle size or stiffness dispersity leads to the discontinuous-continuous transition of the two-dimensional melting. We further find that as long as the melting is continuous the defect concentrations on the boundary between hexatic and liquid phases remain almost constant, accompanied by an almost constant correlation length. These characteristic defect concentrations and correlation length are universal and independent of particle interactions, temperature, and type of particle dispersity, which act as signatures of the continuous two-dimensional melting.

Connecting glass-forming ability of binary mixtures of soft particles to equilibrium melting temperatures.

The glass-forming ability is an important material property for manufacturing glasses and understanding the long-standing glass transition problem. Because of the nonequilibrium nature, it is difficult to develop the theory for it. Here we report that the glass-forming ability of binary mixtures of soft particles is related to the equilibrium melting temperatures. Due to the distinction in particle size or stiffness, the two components in a mixture effectively feel different melting temperatures, leading to a melting temperature gap. By varying the particle size, stiffness, and composition over a wide range of pressures, we establish a comprehensive picture for the glass-forming ability, based on our finding of the direct link between the glass-forming ability and the melting temperature gap. Our study reveals and explains the pressure and interaction dependence of the glass-forming ability of model glass-formers, and suggests strategies to optimize the glass-forming ability via the manipulation of particle interactions.