No Arabic abstract
This paper presents computer simulations of Cu$_x$Zr$_{100-x}$ $(x=36,50,64)$ in the liquid and glass phases. The simulations are based on the effective-medium theory (EMT) potentials. We find good invariance of both structure and dynamics in reduced units along the isomorphs of the systems. The state points studied involve a density variation of almost a factor of two and temperatures going from 1500 K to above 4000 K for the liquids and from 500 K to above 1500 K for the glasses. For comparison, results are presented also for similar temperature variations along isochores, showing little invariance. In general for a binary system the phase diagram has three axes: composition, temperature and pressure (or density). When isomorphs are present, there are effectively only two axes, and for a fixed composition just one. We conclude that the liquid and glass parts of the thermodynamic phase diagram of this metallic glass former at a fixed composition is effectively one-dimensional in the sense that many physical properties are invariant along the same curves, implying that in order to investigate the phase diagram, it is only necessary to go across these curves.
We provide a compact derivation of the static and dynamic equations for infinite-dimensional particle systems in the liquid and glass phases. The static derivation is based on the introduction of an auxiliary disorder and the use of the replica method. The dynamic derivation is based on the general analogy between replicas and the supersymmetric formulation of dynamics. We show that static and dynamic results are consistent, and follow the Random First Order Transition scenario of mean field disordered glassy systems.
The phase stability and equilibria of carbon dioxide is investigated from 125 -- 325K and 1 -- 10,000 atm using extensive molecular dynamics (MD) simulations and the Two-Phase Thermodynamics (2PT) method. We devise a direct approach for calculating phase diagrams in general, by considering the separate chemical potentials of the isolated phase at specific points on the P-T diagram. The unique ability of 2PT to accurately and efficiently approximate the entropy and Gibbs energy of liquids thus allows for assignment of phase boundaries from relatively short ($mathrm{sim}$ 100ps) MD simulations. We validate our approach by calculating the critical properties of the flexible Elementary Physical Model 2 (FEPM2), showing good agreement with previous results. We show, however, that the incorrect description of the short-range Pauli force and the lack of molecular charge polarization leads to deviations from experiments at high pressures. We thus develop a many-body, fluctuating charge model for CO${}_{2}$, termed CO${}_{2}$-Fq, from high level quantum mechanics (QM) calculations, that accurately captures the condensed phase vibrational properties of the solid (including the Fermi resonance at 1378 cm${}^{-1}$) as well as the diffusional properties of the liquid, leading to overall excellent agreement with experiments over the entire phase diagram. This work provides an efficient computational approach for determining phase diagrams of arbitrary systems and underscore the critical role of QM charge reorganization physics in molecular phase stability.
One-dimensional (1D) quantum systems, which are predicted to exhibit novel states of matter in theory, have been elusive in experiment. Here we report a superlattice method of creating artificial 1D quantum stripes, which offers dimensional tunability from two- to one-dimensions. As a model system, we have fabricated 1D iridium (Ir) stripes using a-axis oriented superlattices of a relativistic Mott insulator Sr2IrO4 and a wide bandgap insulator LaSrGaO4, both of which are crystals with layered structure. In addition to the successful formation of 1D Ir-stripe structure, we have observed 1D quantum-confined electronic states from optical spectroscopy and resonant inelastic x-ray scattering. Since this 1D superlattice approach can be applied to a wide range of layered materials, it opens a new era of 1D science.
Nowadays powerful X-ray sources like synchrotrons and free-electron lasers are considered as ultimate tools for probing microscopic properties in materials. However, the correct interpretation of such experiments requires a good understanding on how the beam affects the properties of the sample, knowledge that is currently lacking for intense X-rays. Here we use X-ray photon correlation spectroscopy to probe static and dynamic properties of oxide and metallic glasses. We find that although the structure does not depend on the flux, strong fluxes do induce a non-trivial microscopic motion in oxide glasses, whereas no such dependence is found for metallic glasses. These results show that high fluxes can alter dynamical properties in hard materials, an effect that needs to be considered in the analysis of X-ray data but which also gives novel possibilities to study materials properties since the beam can not only be used to probe the dynamics but also to pump it.
At low temperatures, elementary excitations of a one-dimensional quantum liquid form a gas that can move as a whole with respect to the center of mass of the system. This internal motion attenuates at exponentially long time scales. As a result, in a broad range of frequencies the liquid is described by two-fluid hydrodynamics, and the system supports two sound modes. The physical nature of the two sounds depends on whether the particles forming the quantum liquid have a spin degree of freedom. For particles with spin, the modes are analogous to the first and second sound modes in superfluid $^4$He, which are the waves of density and entropy, respectively. When dissipative processes are taken into account, we find that at low frequencies the second sound is transformed into heat diffusion, while the first sound mode remains weakly damped and becomes the ordinary sound. In a spinless liquid the entropy and density oscillations are strongly coupled, and the resulting sound modes are hybrids of the first and second sound. As the frequency is lowered and dissipation processes become important, the crossover to single-fluid regime occurs in two steps. First the hybrid modes transform into predominantly density and entropy waves, similar to the first and second sound, and then the density wave transforms to the ordinary sound and the entropy wave becomes a heat diffusion mode. Finally, we account for the dissipation due to viscosity and intrinsic thermal conductivity of the gas of excitations, which controls attenuation of the sound modes at high frequencies.