Solid-liquid interface free energy through metadynamics simulations

Abstract

The solid-liquid interface free energy γsl is a key parameter controlling nucleation and growth during solidification and other phenomena. There are intrinsic difficulties in obtaining accurate experimental values, and the previous approaches to compute γsl with atomistic simulations are computationally demanding. We propose a new approach, which is to obtain γsl from a free energy map of the phase transition reconstructed by metadynamics. We apply this to the benchmark case of a Lennard-Jones potential and the results confirm the most reliable data obtained previously. We demonstrate several advantages of our new approach: it is simple to implement, robust and free of hysteresis problems, it allows a rigorous and unbiased estimate of the statistical uncertainty and it returns a good estimate of of the thermodynamic limit with system sizes of a just a few hundred atoms. It is therefore attractive for using with more realistic and specific models of interatomic forces.

arXiv commentimproved version with new figures and tuned metadynamics parameters

References in corpus (9)

• Escaping free-energy minima
• Well-Tempered Metadynamics: A Smoothly Converging and Tunable Free-Energy Method
• An efficient, multiple range random walk algorithm to calculate the density of states
• PLUMED: a portable plugin for free-energy calculations with molecular dynamics
• Equilibrium free energies from non-equilibrium metadynamics
• Direct calculation of the hard-sphere crystal/melt interfacial free energy
• Langevin equation with colored noise for constant-temperature molecular dynamics simulations
• Direct calculation of the crystal-melt interfacial free energies for continuous potentials: Application to the Lennard-Jones system
• Temperature of the inner-core boundary of the Earth: Melting of iron at high pressure from first-principles coexistence simulations

Cited by in corpus (24)

• Crystal Nucleation in Liquids: Open Questions and Future Challenges in Molecular Dynamics Simulations
• Physics-inspired structural representations for molecules and materials
• Unsupervised machine learning in atomistic simulations, between predictions and understanding
• The mold integration method for the calculation of the crystal-fluid interfacial free energy from simulations
• Equilibrium fluid-solid coexistence of hard spheres
• The kinetics of homogeneous melting beyond the limit of superheating
• Crystal-liquid interfacial free energy via thermodynamic integration
• Calculations of excess free energies of precipitates via direct thermodynamic integration across phase boundaries
• Calculation of phase diagrams in the multithermal-multibaric ensemble
• The solid-liquid interfacial free energy out of equilibrium
• Simulation of the carbon dioxide hydrate-water interfacial energy
• Finite-temperature materials modeling from the quantum nuclei to the hot electrons regime
• Equivalence between condensation and boiling in a Lennard Jones fluid
• Computer simulation study of surface wave dynamics at the crystal--melt interface
• Bridging the gap between atomistic and macroscopic models of homogeneous nucleation
• The Gibbs free energy of homogeneous nucleation: from atomistic nuclei to the planar limit
• Direct calculation of the planar NaCl-aqueous solution interfacial free energy at the solubility limit
• Computing the Tolman length for solid-liquid interfaces
• Classical nucleation theory predicts the shape of the nucleus in homogeneous solidification
• Tethered Monte Carlo: Managing rugged free-energy landscapes with a Helmholtz-potential formalism
• Step Free Energies at Faceted Solid-Liquid Interfaces from Equilibrium Molecular Dynamics Simulations
• Rotationally invariant local bond order parameters for accurate determination of hydrate structures
• Predictions of the interfacial free energy along the coexistence line from single-state calculations
• Global free energy landscapes as a smoothly joined collection of local maps