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Register a new userDipolar Dimer Liquid
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Junyi Zhang
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A model of dipolar dimer liquid (DDL) on a two-dimensional lattice has been proposed. We found that at high density and low temperature, it has a partially ordered phase which we called glacia phase. The glacia phase transition can be understood by mapping the DDL to an annealed Ising model on random graphs. In the high density limit the critical temperature obtained by the Monte Carlo simulation is $k_BT_c^G = (3.5pm0.1)J$, which agrees with the estimations of the upper and lower bounds of $k_BT_c^G$ with exactly solved Ising models. In the high density and low temperature limit, we further studied configurational entropy of the DDL in the presence of the neutral polymers. The suppression of the configurational entropy scales as a power law of the polymer length $lambda_p^alpha$ with $alpha geq 1$, which implies that the configurational entropy of water plays essential roles in understanding the hydrophobic effect and the protein folding problem.
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Liquid-liquid phase separation of liquids exhibiting interconversion between alternative states has been proposed as an underlying mechanism for fluid polyamorphism, and may be of relevance to protein function and intracellular organization. However, molecular-level insight into the interplay between competing forces that can drive or restrict phase separation in interconverting fluids remains elusive. Here, we utilize an off-lattice model of enantiomers with tunable chiral interconversion and interaction properties to elucidate the physics underlying the stabilization and tunability of phase separation in fluids with interconverting states. We show that introducing an imbalance in the intermolecular forces between two enantiomers results in nonequilibrium, arrested phase separation into microdomains. We also find that in the equilibrium case, when all interaction forces are conservative, the growth of the phase domain is restricted only by system size. In this case, we observe phase amplification, in which one of the two alternative phases grows at the expense of the other. These findings provide novel insights on how the interplay between dynamics and thermodynamics defines the equilibrium and steady-state morphologies of phase transitions in fluids with interconverting molecular or supramolecular states.
We study the dynamical behavior of a square lattice Ising model with exchange and dipolar interactions by means of Monte Carlo simulations. After a sudden quench to low temperatures we find that the system may undergo a coarsening process where stripe phases with different orientations compete or alternatively it can relax initially to a metastable nematic phase and then decay to the equilibrium stripe phase through nucleation. We measure the distribution of equilibration times for both processes and compute their relative probability of occurrence as a function of temperature and system size. This peculiar relaxation mechanism is due to the strong metastability of the nematic phase, which goes deep in the low temperature stripe phase. We also measure quasi-equilibrium autocorrelations in a wide range of temperatures. They show a distinct decay to a plateau that we identify as due to a finite fraction of frozen spins in the nematic phase. We find indications that the plateau is a finite size effect. Relaxation times as a function of temperature in the metastable region show super-Arrhenius behavior, suggesting a possible glassy behavior of the system at low temperatures.
Spherical truncations of Coulomb interactions in standard models for water permit efficient molecular simulations and can give remarkably accurate results for the structure of the uniform liquid. However truncations are known to produce significant errors in nonuniform systems, particularly for electrostatic properties. Local molecular field (LMF) theory corrects such truncations by use of an effective or restructured electrostatic potential that accounts for effects of the remaining long-ranged interactions through a density-weighted mean field average and satisfies a modified Poissons equation defined with a Gaussian-smoothed charge density. We apply LMF theory to three simple molecular systems that exhibit different aspects of the failure of a naive application of spherical truncations -- water confined between hydrophobic walls, water confined between atomically-corrugated hydrophilic walls, and water confined between hydrophobic walls with an applied electric field. Spherical truncations of 1/r fail spectacularly for the final system in particular, and LMF theory corrects the failings for all three. Further, LMF theory provides a more intuitive way to understand the balance between local hydrogen bonding and longer-ranged electrostatics in molecular simulations involving water.
We demonstrate the accurate calculation of entropies and free energies for a variety of liquid metals using an extension of the two phase thermodynamic (2PT) model based on a decomposition of the velocity autocorrelation function into gas-like (hard sphere) and solid-like (harmonic) subsystems. The hard sphere model for the gas-like component is shown to give systematically high entropies for liquid metals as a direct result of the unphysical Lorentzian high-frequency tail. Using a memory function framework we derive a generally applicable velocity autocorrelation and frequency spectrum for the diffusive component which recovers the low frequency (long time) behavior of the hard sphere model while providing for realistic short time coherence and high frequency tails to the spectrum. This approach provides a significant increase in the accuracy of the calculated entropies for liquid metals and is compared to ambient pressure data for liquid sodium, aluminum, gallium, tin, and iron. The use of this method for the determination of melt boundaries is demonstrated with a calculation of the high pressure bcc melt boundary for sodium. With the significantly improved accuracy available with the memory function treatment for softer interatomic potentials, the 2PT model for entropy calculations should find broader application in high energy density science, warm dense matter, planetary science, geophysics, and material science.
The curvature dependence of interfacial free energy, which is crucial in quantitatively predicting nucleation kinetics and the stability of bubbles and droplets, can be described in terms of the Tolman length {delta}. For solid-liquid interfaces, however,{delta} has never been computed directly due to various theoretical and practical challenges. Here we present a general method that enables the direct evaluation of the Tolman length from atomistic simulations of a solid-liquid planar interface in out-of-equilibrium conditions. This method works by first measuring the surface tension from the amplitude of thermal capillary fluctuations of a localized version of Gibbs dividing surface, and bythen computing the free energy difference between the surface of tension and the equimolar dividing surface. For benchmark purposes, we computed {delta}for a model potential, and compared the results to less rigorous indirect approaches.
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