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Recent advances in classical density functional theory are combined with stochastic process theory and rare event techniques to formulate a theoretical description of nucleation, including crystallization, that can predict nonclassical…

Chemical Physics · Physics 2019-04-09 James F. Lutsko

The expression of the free energy density of a classical crystalline system as a gradient expansion in terms of a set of order parameters is developed using classical density functional theory. The goal here is to extend and complete an…

Statistical Mechanics · Physics 2009-11-11 James F. Lutsko

We investigate the kinetics and the free energy landscape of the crystallization of hard spheres from a supersaturated metastable liquid though direct simulations and forward flux sampling. In this first paper, we describe and test two…

Soft Condensed Matter · Physics 2018-08-17 David Richard , Thomas Speck

In many systems, nucleation of a stable solid may occur in the presence of other (often more than one) metastable phases. These may be polymorphic solids or even liquid phases. In such cases, nucleation of the solid phase from the melt may…

Materials Science · Physics 2013-04-08 Mantu Santra , Rakesh S. Singh , Biman Bagchi

We investigate the crystal structure of classical systems of spherical particles with an embedded point dipole at T=0. The ferroelectric ground state energy is calculated using generalizations of the Ewald summation technique. Due to the…

Soft Condensed Matter · Physics 2009-10-31 B. Groh , S. Dietrich

While in principle, finite temperature density functional theory (ftDFT) should be a powerful tool for the study of crystallization, in practice this has not so far been the case. Progress has been hampered by technical problems which have…

Soft Condensed Matter · Physics 2018-07-16 James F. Lutsko , Julien Lam

Classical density-functional theory provides an efficient alternative to molecular dynamics simulations for understanding the equilibrium properties of inhomogeneous fluids. However, application of density-functional theory to multi-site…

Computational Physics · Physics 2014-02-14 Ravishankar Sundararaman , T. A. Arias

Using a generalized order parameter gradient expansion within density functional theory, we derive a phase-field-crystal model for liquid crystals composed by apolar particles in three spatial dimensions. Both the translational density and…

Soft Condensed Matter · Physics 2014-01-28 Raphael Wittkowski , Hartmut Löwen , Helmut R. Brand

By combining methods of kinetic and density functional theory, we present a description of molecular fluids which accounts for their microscopic structure and thermodynamic properties as well as for the hydrodynamic behavior. We focus on…

Mesoscale and Nanoscale Physics · Physics 2015-05-18 Umberto Marini Bettolo Marconi , Simone Melchionna

Previously, it has been shown that the direct correlation function for a Lennard-Jones fluid could be modeled by a sum of that for hard-spheres, a mean-field tail and a simple linear correction in the core region constructed so as to…

Statistical Mechanics · Physics 2008-08-20 James F. Lutsko

The role of metastable liquid phases in vapor-crystal nucleation is studied using Density Functional Theory(DFT). The model gives a semi-quantitatively accurate description of both the vapor-liquid-solid phase diagram for both simple fluids…

Soft Condensed Matter · Physics 2015-03-19 James F. Lutsko

We present an isothermal fluctuating nonlinear hydrodynamic theory of crystallization in molecular liquids. A dynamic coarse-graining technique is used to derive the velocity field, a phenomenology, which allows a direct coupling between…

Materials Science · Physics 2013-10-15 Gyula I. Tóth , László Gránásy , György Tegze

We present a computer simulation study of a (6,12)-Lennard-Jones fluid confined to a slit pore, formed by two uniform planes. These interact via (3,9)-Lennard-Jones potential with the fluid particles. When the fluid approaches the…

Soft Condensed Matter · Physics 2009-02-20 N. Gribova , H. Maleki , A. Arnold , C. Holm , T. Schilling

Recently, it was shown that a theoretical description of nucleation based on fluctuating hydrodynamics and classical density functional theory can be used to determine non-classical nucleation pathways for crystallization (Lutsko, Sci. Adv.…

Chemical Physics · Physics 2024-06-26 James F. Lutsko , Cédric Schoonen

Understanding the pathways to crystallization during the deposition of a vapor phase on a cold solid substrate is of great interest in industry, e.g., for the realization of electronic devices made of crystallites-free glassy materials, as…

Soft Condensed Matter · Physics 2023-10-03 Fabio Leoni , Hajime Tanaka , John Russo

Non-aligning self-propelled particles with purely repulsive excluded volume interactions undergo athermal motility-induced phase separation into a dilute gas and a dense cluster phase. Here, we use enhanced sampling computational methods…

Soft Condensed Matter · Physics 2016-10-05 Gabriel S. Redner , Caleb G. Wagner , Aparna Baskaran , Michael F. Hagan

We discuss the growth process of a crystalline phase out of a metastable over-compressed liquid that is brought into contact with a crystalline substrate. The process is modeled by means of molecular dynamics. The particles interact via the…

Soft Condensed Matter · Physics 2014-08-07 Francesco Turci , Tanja Schilling

We report on a large scale computer simulation study of crystal nucleation in hard spheres. Through a combined analysis of real and reciprocal space data, a picture of a two-step crystallization process is supported: First dense, amorphous…

Soft Condensed Matter · Physics 2015-05-18 T. Schilling , H. J. Schope , M. Oettel , G. Opletal , I. Snook

We use machine learning methods to approximate a classical density functional. As a study case, we choose the model problem of a Lennard Jones fluid in one dimension where there is no exact solution available and training data sets must be…

Soft Condensed Matter · Physics 2019-03-04 Shang-Chun Lin , Martin Oettel

The process of nucleation of vapor bubbles from a superheated liquid and of liquid droplets from a supersaturated vapor is investigated using the Modified-Core van der Waals model Density Functional Theory (Lutsko, JCP 128, 184711 (2008)).…

Statistical Mechanics · Physics 2009-11-13 James F. Lutsko
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