Fundamental-measure density functional theory study of the crystal-melt interface of the hard sphere system

Warshavsky, Vadim B.; Song, Xueyu

doi:10.1103/physreve.73.031110

Cited by 22 publications

(29 citation statements)

References 36 publications

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“…is a similar order of magnitude to previously found values of ␥ for hard spheres, which range from 0.11 to 0.78 (8,9,12,(22)(23)(24). Our measured ␥ is larger than these values of ␥, perhaps due to the above-noted anisotropy of ␥, for which we may have a stiff direction (8).…”

Section: Resultscontrasting

confidence: 41%

The equilibrium intrinsic crystal–liquid interface of colloids

Hernandez-Guzman

Weeks

2009

Proc. Natl. Acad. Sci. U.S.A.

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We use confocal microscopy to study an equilibrated crystal-liquid interface in a colloidal suspension. Capillary waves roughen the surface, but locally the intrinsic interface is sharply defined. We use local measurements of the structure and dynamics to characterize the intrinsic interface, and different measurements find slightly different widths of this interface. In terms of the particle diameter d, this width is either 1.5d (based on structural information) or 2.4d (based on dynamics), both not much larger than the particle size. This work is the first direct experimental visualization of an equilibrated crystal-liquid interface.surface tension ͉ capillary waves ͉ confocal microscopy T he interface between crystal and liquid phases of a material governs phenomena such as wetting, lubrication, and crystal nucleation (1, 2). Interfaces are poorly defined at the atomic level: Capillary waves cause fluctuations in the interface position (3-6), and locally the structure varies in a smooth way from ordered to disordered (2). Existing literature makes a distinction between the intrinsic interface (presumed to be sharp) (3), and the observed surface blurred by capillary waves (4, 7). The standard equilibrium interface profile is well defined and contains fluctuations at all length and time scales, due to these capillary waves. Because of the rapid time scales of capillarywave fluctuations, along with the small length scales at the interface, it is difficult to study these interfaces directly (1). Thus, computer simulations provide useful information about model crystal-liquid interfaces, such as hard-sphere systems (2,8,9) and Lennard-Jones systems (10, 11).Recently, crystal-liquid interfaces were directly studied in colloidal suspensions by using confocal microscopy (6, 12). Colloids are systems of solid particles in a liquid and are a good model system for phase transitions (5,6,13,14). Microscopy allows direct observation of structure and dynamics of the colloidal particles (15). However, the previous experiments focused on nonequilibrium cases where samples were crystallizing and did not provide data on equilibrium interfaces, such as those studied by simulation (2,(8)(9)(10)16). Furthermore, these experiments did not examine the intrinsic interface, perhaps because they were nonequilibrium studies, and thus crystalline particles were present in the ''liquid'' side and vice versa, which confuse the structure near the interface.In this work, we present confocal microscope observations of an equilibrated colloidal crystal-liquid interface. By following the positions of several thousand colloidal particles on both sides of the interface, we directly visualize the interface. An example of our data is shown in Fig. 1A, where blue particles are crystalline and yellow/red particles are liquid-like. This interface has a low surface tension, and we see capillary waves. We are able to remove the influence of these capillary waves from the data and measure the intrinsic surface profile. In particular, we find that capill...

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Section: Resultscontrasting

confidence: 41%

The equilibrium intrinsic crystal–liquid interface of colloids

Hernandez-Guzman

Weeks

2009

Proc. Natl. Acad. Sci. U.S.A.

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“…This introduces some uncertainty as to the precision for the value of the interfacial tension since the functional minimization is constrained. Depending on the particular FMT functional the interfacial tension is close [7] or 25% above [8] corresponding simulation values. In Section 3 we discuss the hard sphere crystal-liquid interface in more detail and present also results of unconstrained minimizations.…”

Section: Density Functional Theorymentioning

confidence: 99%

“…Previous studies of the crystal-liquid interface in FMT involved restricted parametrizations of the three-dimensional density profile across the interface [7,8]. This introduces some uncertainty as to the precision for the value of the interfacial tension since the functional minimization is constrained.…”

Section: Density Functional Theorymentioning

confidence: 99%

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Solid phase properties and crystallization in simple model systems

Turci

Schilling

Yamani

et al. 2014

Eur. Phys. J. Spec. Top.

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Abstract. We review theoretical and simulational approaches to the description of equilibrium bulk crystal and interface properties as well as to the nonequilibrium processes of homogeneous and heterogeneous crystal nucleation for the simple model systems of hard spheres and Lennard-Jones particles. For the equilibrium properties of bulk and interfaces, density functional theories employing fundamental measure functionals prove to be a precise and versatile tool, as exemplified with a closer analysis of the hard sphere crystal-liquid interface. A detailed understanding of the dynamic process of nucleation in these model systems nevertheless still relies on simulational approaches. We review bulk nucleation and nucleation at structured walls and examine in closer detail the influence of walls with variable strength on nucleation in the Lennard-Jones fluid. We find that a planar crystalline substrate induces the growth of a crystalline film for a large range of lattice spacings and interaction potentials. Only a strongly incommensurate substrate and a very weakly attractive substrate potential lead to crystal growth with a non-zero contact angle.

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“…For temperature * = / =2.74, the excess free energy per particle = − ln( 3 ) + 1 is compared with the MC results [1][2][3][4] in Table 3. …”

Section: Results Of Liquid Free Energy Of Lj Systemmentioning

confidence: 99%

Perturbation theory calculations of model pair potential systems

Gong

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Fundamental-measure density functional theory study of the crystal-melt interface of the hard sphere system

Cited by 22 publications

References 36 publications

The equilibrium intrinsic crystal–liquid interface of colloids

The equilibrium intrinsic crystal–liquid interface of colloids

Solid phase properties and crystallization in simple model systems

Perturbation theory calculations of model pair potential systems

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