We use molecular simulations to study the early stages of crystallization in a supercooled liquid Lennard-Jones particles. observe onset concomitant polymorphism and demonstrate that this phenomenon results from cross-nucleation metastable polymorph on stable polymorph. also show is selective as it only takes place between polymorphs almost equivalent free energy. Our provide detailed insights into mechanism underlying polymorphs.

We use molecular dynamics simulations to shed light on polymorph selection during the crystallization of Lennard-Jones fluid. By varying pressure at fixed supercooling, we form large crystallites either stable face centered cubic or metastable body and even fine-tune fractions polymorphs in crystallite. demonstrate that conditions crystallization, leading bcc crystallites, lie within occurrence domain polymorph. also find predominantly fcc contain a notable amount hexagonal close packed...

We use molecular simulations to study polymorph selection during the crystallization of charge-stabilized colloidal suspension. By modifying conditions crystallization, we invert stability two polymorphs and induce formation crystallites whose structure is predominantly that stable polymorph. However, our reveal kinetics play a major role not only nucleation step but also in growth mechanism. The postcritical proceeds through complex mechanism involving cross-nucleation third metastable...

We use molecular simulations to study the onset of crystallization in a liquid Al, cooled at temperature 20% below melting point. show that Al nucleates into random packing hexagonal close-packed and face-centered cubic phases. Body-centered clusters, which usually form during nucleation simple fluids, are not observed Al. Throughout growth, nuclei always strongly faceted, sharp contrast with spherical crystallites for fluids. Our results demonstrate pathway departs from

The Wang-Landau sampling is a powerful method that allows for direct determination of the density states. However, applications to calculation thermodynamic properties realistic fluids have been limited so far. By combining with expanded grand-canonical simulations, we obtain high-accuracy estimate partition function atomic and molecular fluids. Then, using formalism statistical thermodynamics, are able calculate these systems, wide range conditions spanning single-phase regions as well...

In recent years, powerful and accurate methods, based on a Wang-Landau sampling, have been developed to determine phase equilibria. However, while these methods extensively applied study the behavior of model fluids, they yet be molecular systems. this work, we show how, by combining hybrid Monte Carlo simulations in isothermal-isobaric ensemble with sampling method, vapor-liquid equilibria various fluids. More specifically, present results obtained rigid molecules, such as benzene, well...

We propose to apply expanded Wang-Landau simulations study the adsorption of atomic and molecular fluids in porous materials. This approach relies on a uniform sampling number atoms molecules adsorbed. The method consists determining high-accuracy estimate grand-canonical partition function for adsorbed fluids. Then, using formalism statistical mechanics, we calculate absolute excess thermodynamic properties relevant processes. In this paper, examine argon carbon dioxide isoreticular...

Using molecular simulation, we establish the pivotal role played by liquid polymorphs during crystallization of silicon. When undercooled at a temperature 20% below melting point, silicon melt is under form highly coordinated, high-density (HDL) polymorph. We find that starts with formation, within HDL liquid, nanosized droplet least stable polymorph, known as almost tetracoordinated low-density (LDL) then show crystalline embryo forms LDL droplet, close to interface surrounding thereby...

Combining rules, such as the Lorentz-Berthelot are routinely used to calculate thermodynamic properties of mixtures using molecular simulations. Here we extend expanded Wang-Landau simulation approach determine impact combining rules on value partition function binary systems, and, in turn, phase coexistence and thermodynamics these mixtures. We study various types mixtures, ranging from systems rare gases biologically technologically relevant water-urea water-carbon dioxide. Comparing...

Using molecular simulations, we shed light on the mechanism underlying crystal nucleation in metal alloys and unravel interplay between glass transition, as conditions of crystallization lie close to this transition. While decreasing temperature usually results a lower free energy barrier, find an unexpected reversal behavior for glass-forming approaches For purpose, simulate process two Copper alloys, Ag_{6}Cu_{4}, which has positive heat mixing, CuZr, characterized by large negative...

Using molecular-dynamics simulations, we study the crystallization of supercooled liquids charge-stabilized colloidal suspensions, modeled by Yukawa (screened-Coulomb) potential. By modifying value screening parameter λ, are able to invert stability body-centered cubic (bcc) and face-centered (fcc) polymorphs crystal nucleation growth in domain each polymorph. We show that mechanism strongly depends on λ. When bcc is stable polymorph (λ=3), straightforward. Both kinetics thermodynamics favor...

Using hybrid Monte Carlo as well molecular dynamics simulation, we study the nucleation and growth of nanoparticles from a supercooled liquid Au at ambient pressure. We simulate step using an umbrella sampling scheme in course simulations. then monitor subsequent critical nuclei so obtained. In particular, carefully determine kinetics mechanisms underlying step. Our results establish following crystallization pathway. early stages process, structure nucleus is dominated by stable...

We report hybrid Monte Carlo molecular simulation results on the crystallization of aluminum from supercooled liquid. simulate entire process at P=1atm and temperatures 20% 15% below melting temperature. demonstrate that takes place according to same mechanism for two degrees supercooling considered in this work. show both nucleation growth proceed into a random mixing hexagonal close packed structure face centered cubic (fcc) phase, with predominance stable fcc form. The concentration...

We report hybrid Monte Carlo molecular simulation results on the crystallization of supercooled liquids xenon at high temperature and pressure. simulate entire process, i.e., nucleation event as well subsequent growth critical nucleus, $P=4.46\phantom{\rule{0.3em}{0ex}}\mathrm{GPa}$ $P=87.96\phantom{\rule{0.3em}{0ex}}\mathrm{GPa}$. In both cases, we carry out simulations a 25% below melting temperature. demonstrate that mechanism strongly depends At...

The determination of the critical parameters metals has remained particularly challenging both experimentally, because very large temperatures involved, and theoretically, many-body interactions that take place in metals. Moreover, experiments have shown these systems exhibit an unusually strong asymmetry their binodal. Recent theoretical work led to new similarity laws, based on calculation Zeno line underlying Boyle parameters, which provided results for properties atomic molecular...

Crystallization often proceeds through successive stages that lead to a gradual increase in organization. Using molecular simulation, we determine the nucleation pathway for solid solutions of copper and gold. We identify new mechanism (liquid$\to$$L1_2$~precursor$\to$solid solution), involving chemically ordered intermediate is more organized than end product. This arises from low formation energy $L1_2$ clusters which, turn, promote crystal nucleation. also show this composition-dependent...

Using Expanded Wang–Landau simulations, we have determined with great accuracy the grand-canonical partition function of CO2 adsorbed in IRMOF-1, IRMOF-8, and IRMOF-10. Then, following a solution thermodynamics approach to adsorption, use so obtained calculate immersion desorption free energy, enthalpy, entropy, which provide complete thermodynamic characterization three systems. Excess functions are found be monotonic pressure subcritical regime present an extremum supercritical regime....

Using molecular simulation, we shed light on the coupling between two nonequilibrium processes of demixing and crystallization in mixtures fully miscible, size-matched, liquid metals. We show that competition these has a strong impact pathway, leading to formation crystal nuclei with large excesses (up 95%) component higher cohesive energy, resulting increases more than 30% free energy barrier nucleation. The goes growth process, as shown by variations composition observed at surface inside...

We review recent advances in the design, synthesis, and modeling of active fluids. Active fluids have been at center many technological innovations theoretical over past two decades. Research on this new class has inspired by fascinating remarkably efficient strategies that biological systems employ, leading to development biomimetic nano- micro-machines -swimmers. The encompasses both micro-scale. start with examples before we discuss how experimentalists leverage novel propulsion...

Using classical molecular dynamics simulations together with a many-body embedded atom model (EAM) potential, we calculate the viscosity of liquid iron under high temperature and pressure. We show that this EAM in addition to reproducing experimental data on structure at pressure, accurately predicts shear iron. carefully assess validity our results, obtained from equilibrium as well nonequilibrium simulations. Our estimates for are shown be good agreement those ab initio This demonstrates...

Using classical molecular dynamics simulation together with the quantum-corrected Sutton-Chen many-body embedded-atom model, we study rheology of several liquid fcc metals (Pb, Pt, Ir, Ag, and Rh) at ambient pressure four temperatures ranging from 5% below melting temperature to 75% above temperature. We first carry out equilibrium simulations determine, using Green-Kubo's formalism, shear viscosity ${\ensuremath{\eta}}_{\text{GK}}$, modulus ${G}_{\ensuremath{\infty}}$, Maxwell relaxation...