Nucleation instability in supercooled Cu-Zr-Al glass-forming liquids.

Few general models representing certain classes of real glass-forming systems play a special role in computer simulations of supercooled liquid and glasses. Recently, it was shown that one of the most widely used model glassformers-the Kob-Andersen binary mixture-crystalizes in quite lengthy molecular dynamics simulations, and moreover, it is in fact a very poor glassformer at large system sizes. Thus, our understanding of crystallization stability of model glassformers is far from complete due to the fact that relatively small system sizes and short time scales have been considered so far. Here we address this issue for two embedded atom models intensively used last years in numerical studies of Cu-Zr-(Al) bulk metallic glasses. Exploring the structural evolution of Cu64.5Zr35.5 and Cu46Zr46Al8 alloys at continuous cooling and isothermal annealing, we observe that both systems nucleate in sufficiently lengthy simulations, although critical nucleation time for the latter is an order of magnitude higher than that for the former. We show that Cu64.5Zr35.5 is actually unstable to crystallization for large system sizes (N > 20 000). Both systems crystallize with the formation of tetrahedrally close packed Laves phases of different types. We argue that nucleation instability of the simulated Cu64.5Zr35.5 alloy is due to the fact that its composition is very close to that for the stable Cu2Zr compound with a C15 Laves phase structure.

Polytetrahedral structure and glass-forming ability of simulated Ni-Zr alloys.

Binary Cu-Zr system is a representative bulk glassformer demonstrating high glass-forming ability (GFA). From the first glance, the Ni-Zr system is the most natural object to expect the same behavior because nickel and copper are neighbors in the periodic table and have similar physicochemical properties. However, it is known that the Ni-Zr system has worse GFA than the Cu-Zr one. To understand the underlying physics, we investigate the Ni α Zr1-α system in whole concentration range α ∈ [0, 1]. Doing molecular dynamic simulations with a reliable embedded atom model potential, we show that the simulated Ni-Zr system also has relatively low GFA, which is comparable to that for an additive binary Lennard-Jones mixture without any chemical interaction. Icosahedral local ordering in Ni-Zr alloys is known to be less pronounced than that in the Cu-Zr ones; we see that as well. However, the icosahedron is not the only structural motif responsible for GFA. We find that the local structure of glassy Ni α Zr1-α alloys at 0.3 < α < 0.65 can be described in terms of Z11-Z16 Kasper polyhedra with high density of topological defects including icosahedra as a part of this family. Concentration of topologically perfect Kasper polyhedra appears to be several times smaller than that in Cu-Zr. This is the reason for relatively poor GFA of the Ni-Zr system.

Cooling rate dependence of simulated Cu64.5Zr35.5 metallic glass structure.

Using molecular dynamics simulations with embedded atom model potential, we study structural evolution of Cu64.5Zr35.5 alloy during the cooling in a wide range of cooling rates γ ∈ (1.5 ⋅ 10(9), 10(13)) K/s. Investigating short- and medium-range orders, we show that the structure of Cu64.5Zr35.5 metallic glass essentially depends on cooling rate. In particular, a decrease of the cooling rate leads to an increase of abundances of both the icosahedral-like clusters and Frank-Kasper Z16 polyhedra. The amounts of these clusters in the glassy state drastically increase at the γmin = 1.5 ⋅ 10(9) K/s. Analysing the structure of the glass at γmin, we observe the formation of nano-sized crystalline grain of Cu2Zr intermetallic compound with the structure of Cu2Mg Laves phase. The structure of this compound is isomorphous with that for Cu5Zr intermetallic compound. Both crystal lattices consist of two types of clusters: Cu-centered 13-atom icosahedral-like cluster and Zr-centered 17-atom Frank-Kasper polyhedron Z16. That suggests the same structural motifs for the metallic glass and intermetallic compounds of Cu-Zr system and explains the drastic increase of the abundances of these clusters observed at γmin.

How to quantify structural anomalies in fluids?

Some fluids are known to behave anomalously. The so-called structural anomaly which means that the fluid becomes less structures under isothermal compression is among the most frequently discussed ones. Several methods for quantifying the degree of structural order are described in the literature and are used for calculating the region of structural anomaly. It is generally thought that all of the structural order determinations yield qualitatively identical results. However, no explicit comparison was made. This paper presents such a comparison for the first time. The results of some definitions are shown to contradict the intuitive notion of a fluid. On the basis of this comparison, we show that the region of structural anomaly can be most reliably determined from the behavior of the excess entropy.

Geometric frustration of icosahedron in metallic glasses.

Icosahedral order has been suggested as the prevalent atomic motif of supercooled liquids and metallic glasses for more than half a century, because the icosahedron is highly close-packed but is difficult to grow, owing to structure frustration and the lack of translational periodicity. By means of angstrom-beam electron diffraction of single icosahedra, we report experimental observation of local icosahedral order in metallic glasses. All the detected icosahedra were found to be distorted with partially face-centered cubic symmetry, presenting compelling evidence on geometric frustration of local icosahedral order in metallic glasses.

Fluid-solid phase transitions in three-dimensional complex plasmas under microgravity conditions.

Phase behavior of large three-dimensional (3D) complex plasma systems under microgravity conditions onboard the International Space Station is investigated. The neutral gas pressure is used as a control parameter to trigger phase changes. Detailed analysis of structural properties and evaluation of three different melting-freezing indicators reveal that complex plasmas can exhibit melting by increasing the gas pressure. Theoretical estimates of complex plasma parameters allow us to identify main factors responsible for the observed behavior. The location of phase states of the investigated systems on a relevant equilibrium phase diagram is estimated. Important differences between the melting process of 3D complex plasmas under microgravity conditions and that of flat 2D complex plasma crystals in ground based experiments are discussed.

Freezing and melting of 3D complex plasma structures under microgravity conditions driven by neutral gas pressure manipulation.

Freezing and melting of large three-dimensional complex plasmas under microgravity conditions is investigated. The neutral gas pressure is used as a control parameter to trigger the phase changes: Complex plasma freezes (melts) by decreasing (increasing) the pressure. The evolution of complex plasma structural properties upon pressure variation is studied. Theoretical estimates allow us to identify the main factors responsible for the observed behavior.

Critical fluctuations and anomalous transport in soft Yukawa-Langevin systems.

Simulation of a Langevin-dynamics model demonstrates emergence of critical fluctuations and anomalous grain transport which have been observed in experiments on "soft" quasi-two-dimensional dusty plasma clusters. Our model does not contain external drive or plasma interactions that serve to drive the system away from thermodynamic equilibrium. The grains are confined by an external potential, interact via static Yukawa forces, and are subject to stochastic heating and dissipation from neutrals. One remarkable feature is emergence of leptokurtic probability distributions of grain displacements xi(tau) on time scales tau < tau(Delta), where tau(Delta) is the time at which the standard deviation sigma(tau) identical with (xi(2)(tau))(1/2) approaches the mean intergrain distance Delta. Others are development of humps in the distributions on multiples of Delta , anomalous Hurst exponents, and transitions from leptokurtic toward Gaussian displacement distributions on time scales tau > tau(Delta). The latter is a signature of intermittency, here interpreted as a transition from bursty transport associated with hopping on intermediate time scales to vortical flows on longer time scales. These intermittency features are quantitatively modeled by a single-particle Itô-Langevin stochastic equation with a nonlinear drift term.

Structural properties of complex plasmas in a homogeneous dc discharge.

We report on the first three-dimensional (3D) complex plasma structure analysis for an experiment that was performed in an elongated discharge tube in the absence of striations. The low frequency discharge was established with 1 kHz alternating dc current through a cylindrical glass tube filled with neon at 30 Pa. The injected particle cloud consisted of monodisperse microparticles. A scanning laser sheet and a camera were used to determine the particle position in 3D. The observed cylindrical-shaped particle cloud showed an ordered structure with a distinct outer particle shell. The observations are in agreement with performed molecular dynamics simulations.

Electric potential around an absorbing body in plasmas: effect of ion-neutral collisions.

A simple linear kinetic model is used to investigate the combined effect of plasma absorption and ion-neutral collisions on the electric potential around a small absorbing body in weakly ionized plasmas. It is demonstrated that far from the body the potential decays considerably slower than the conventional Debye-Hückel potential. Moreover, at distances exceeding approximately the ion mean free path, the potential approaches an unscreened Coulomb-like asymptote. Some important consequences of this result are discussed in the context of complex (dusty) plasmas.

Kinetic characterization of strongly coupled systems.

We propose a simple method to determine the local coupling strength Gamma experimentally, by linking the individual particle dynamics with the local density and crystal structure of a 2D plasma crystal. By measuring particle trajectories with high spatial and temporal resolution we obtain the first maps of Gamma and temperature at individual particle resolution. We employ numerical simulations to test this new method, and discuss the implications to characterize strongly coupled systems.

Kinetics of ensembles with variable charges.

Kinetics of particle ensembles with variable charges is investigated. It is shown that the energy of such ensembles is not conserved in the interparticle collisions. The case when the equilibrium charge depends on the particle coordinate is studied, and the collision integral describing the momentum and energy transfer in collisions is derived. Solution of the resulting kinetic equation shows that the system is unstable--the mean thermal energy exhibits explosion-like growth, diverging at a finite time.