Free Energy Barriers for Crystal Nucleation from Fluid Phases

Monte Carlo simulations of crystal nuclei coexisting with the fluid phase in thermal equilibrium in finite volumes are presented and analyzed, for fluid densities from dense melts to the vapor. Generalizing the lever-rule for two-phase coexistence in the canonical ensemble to finite volume, "measurements" of the nucleus volume together with the pressure and chemical potential of the surrounding fluid allows to extract the surface free energy of the nucleus. Neither the knowledge of the (in general non-spherical) nucleus shape nor of the angle-dependent interface tension is required for this task. The feasibility of the approach is demonstrated for a variant of the Asakura-Oosawa model for colloid-polymer mixtures, which form face-centered cubic colloidal crystals. For a polymer to colloid size ratio of $0.15$, the colloid packing fraction in the fluid phase can be varied from melt values to zero by the variation of an effective attractive potential between the colloids. It is found that the approximation of spherical crystal nuclei often underestimates actual nucleation barriers significantly. Nucleation barriers are found to scale as $\Delta F^*=(4\pi/3)^{1/3}\bar{\gamma}(V^*)^{2/3}+const.$ with the nucleus volume $V^*$, and the effective surface tension $\bar{\gamma}$ that accounts implicitly for the nonspherical shape can be precisely estimated.Comment: 17 pages, 17 figure

Stability of force-driven shear flows in nonequilibrium molecular simulations with periodic boundaries

We analyze the hydrodynamic stability of force-driven parallel shear flows in nonequilibrium molecular simulations with three-dimensional periodic boundary conditions. We show that flows simulated in this way can be linearly unstable, and we derive an expression for the critical Reynolds number as a function of the geometric aspect ratio of the simulation domain. Approximate periodic extensions of Couette and Poiseuille flows are unstable at Reynolds numbers two orders of magnitude smaller than their aperiodic equivalents because the periodic boundaries impose fundamentally different constraints on the flow. This instability has important implications for simulating shear rheology and for designing nonequilibrium simulation methods that are compatible with periodic boundary conditions.Comment: 10 pages, 6 figure

NMR evidence for Friedel-like oscillations in the CuO chains of ortho-II YBa2_2Cu3_3O6.5_{6.5}

Nuclear magnetic resonance (NMR) measurements of CuO chains of detwinned Ortho-II YBa$_2$Cu$_3$O$_{6.5}$ (YBCO6.5) single crystals reveal unusual and remarkable properties. The chain Cu resonance broadens significantly, but gradually, on cooling from room temperature. The lineshape and its temperature dependence are substantially different from that of a conventional spin/charge density wave (S/CDW) phase transition. Instead, the line broadening is attributed to small amplitude static spin and charge density oscillations with spatially varying amplitudes connected with the ends of the finite length chains. The influence of this CuO chain phenomenon is also clearly manifested in the plane Cu NMR.Comment: 4 pages, 3 figures, refereed articl

Weak pseudogap in crystals of Pb2Sr2(Y,Ca)Cu3O8+d

We report on NMR measurements in underdoped Pb2Sr2(Y,Ca)Cu3O8+d crystals. A pseudogap is observed in the Knight shift and spin-lattice relaxation rate. In contrast to other underdoped compounds, the pseudogap observed in the Knight shift is weak and occurs at a significantly lower temperature. On the other hand, the effect the pseudogap has on spin-lattice relaxation is quite similar to that in other compounds. The contrast between weak and strong pseudogaps is discussed.Comment: 4 pages, 3 figures, submitted to PR

The Effects of Phase Separation in the Cuprate Superconductors

Phase separation has been observed by several different experiments and it is believed to be closely related with the physics of cuprates but its exactly role is not yet well known. We propose that the onset of pseudogap phenomenon or the upper pseudogap temperature $T^*$ has its origin in a spontaneous phase separation transition at the temperature $T_{ps}=T^*$. In order to perform quantitative calculations, we use a Cahn-Hilliard (CH) differential equation originally proposed to the studies of alloys and on a spinodal decomposition mechanism. Solving numerically the CH equation it is possible to follow the time evolution of a coarse-grained order parameter which satisfies a Ginzburg-Landau free-energy functional commonly used to model superconductors. In this approach, we follow the process of charge segregation into two main equilibrium hole density branches and the energy gap normally attributed to the upper pseudogap arises as the free-energy potential barrier between these two equilibrium densities below $T_{ps}$. This simulation provides quantitative results %on the hole doping and temperature %dependence of the degree of the charge inhomogeneity in agreement with %some experiments and the simulations reproduce the observed stripe and granular pattern of segregation. Furthermore, with a Bogoliubov-deGennes (BdG) local superconducting critical temperature calculation for the lower pseudogap or the onset of local superconductivity, it yields novel interpretation of several non-conventional measurements on cuprates.Comment: Published versio