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Register a new userPredicting crystal structures: the Parrinello-Rahman method revisited
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By suitably adapting a recent approach [A. Laio and M. Parrinello, PNAS, 99, 12562 (2002)] we develop a powerful molecular dynamics method for the study of pressure-induced structural transformations. We use the edges of the simulation cell as collective variables. In the space of these variables we define a metadynamics that drives the system away from the local minimum towards a new crystal structure. In contrast to the Parrinello-Rahman method our approach shows no hysteresis and crystal structure transformations can occur at the equilibrium pressure. We illustrate the power of the method by studying the pressure-induced diamond to simple hexagonal phase transition in a model of silicon.
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Free energy of crystal phases is commonly evaluated by thermodynamic integration (TDI) along a reversible path that involves an external potential. A persistent problem in this method is that a significant hysteresis is observed due to differences in the center of mass position of the crystal phase in the presence and absence of the external potential. To alleviate this hysteresis, a constraint on the translational degrees of freedom of the crystal phase is imposed along the path and subsequently a correction term is added to the free energy to account for such a constraint. In this work, we propose a new methodology termed as error-biased Bennett Acceptance ratio (EBAR) method that effectively solves this problem without the need to impose any constraint. This method is simple to implement as it does not require any modification to the path or to the simulation code. We show the applicability of this method in the computation of crystal-melt interfacial energy by cleaving wall method [J. Chem. Phys., 118, 7651 (2003)] and bulk crystal-melt free energy difference by constrained fluid $lambda$-integration method [J. Chem. Phys., 120, 2122 (2004)] for a model potential of silicon.
The finite size and interface effects on equilibrium crystal shape (ECS) have been investigated for the case of a surface free energy density including step stiffness and inverse-square step-step interactions. Explicitly including the curvature of a crystallite leads to an extra boundary condition in the solution of the crystal shape, yielding a family of crystal shapes, governed by a shape parameter c. The total crystallite free energy, including interface energy, is minimized for c=0, yielding in all cases the traditional PT shape (z x3/2). Solutions of the crystal shape for c≠0 are presented and discussed in the context of meta-stable states due to the energy barrier for nucleation. Explicit scaled relationships for the ECS and meta-stable states in terms of the measurable step parameters and the interfacial energy are presented.
Analysis of the intriguing physical properties of the dodecaborides, $R$B$_{12}$, requires accurate data on their crystal structure. We show that a simple cubic model fits well with the atomic positions in the unit cell but cannot explain the observed anisotropy in the physical properties. The cooperative Jahn-Teller (JT) effect slightly violates the ideal metric of the cubic lattice and the symmetry of the electron density distribution in the lattice interstices. Theoretical models of the JT distortions of the boron framework are presented. Their correspondence to the electron-density distribution on the maps of Fourier syntheses obtained using x-ray data and explaining the previously observed anisotropy of conductive properties is demonstrated. The effect of boron isotope composition on the character of the lattice distortions is shown. We also discuss the application of the Einstein model for cations and the Debye model for the boron atoms to describe the dynamics of the crystal lattice.
We formulate the problem of probabilistic predictions of global failure in the simplest possible model based on site percolation and on one of the simplest model of time-dependent rupture, a hierarchical fiber bundle model. We show that conditioning the predictions on the knowledge of the current degree of damage (occupancy density $p$ or number and size of cracks) and on some information on the largest cluster improves significantly the prediction accuracy, in particular by allowing to identify those realizations which have anomalously low or large clusters (cracks). We quantify the prediction gains using two measures, the relative specific information gain (which is the variation of entropy obtained by adding new information) and the root-mean-square of the prediction errors over a large ensemble of realizations. The bulk of our simulations have been obtained with the two-dimensional site percolation model on a lattice of size $L times L=20 times 20$ and hold true for other lattice sizes. For the hierarchical fiber bundle model, conditioning the measures of damage on the information of the location and size of the largest crack extends significantly the critical region and the prediction skills. These examples illustrate how on-going damage can be used as a revelation of both the realization-dependent pre-existing heterogeneity and the damage scenario undertaken by each specific sample.
We examine the atomistic scale dependence of materials resistance-to-failure by numerical simulations and analytical analysis in electrical analogs of brittle crystals. We show that fracture toughness depends on the lattice geometry in a way incompatible with Griffiths relationship between fracture and free surface energy. Its value finds its origin in the matching between the continuum displacement field at the engineering scale, and the discrete nature of solids at the atomic scale. The generic asymptotic form taken by this field near the crack tip provides a solution for this matching, and subsequently a way to predict toughness from the atomistic parameters with application to graphene.
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