相关论文: Automated Prediction of Thermodynamic Properties v…

We devise automated workflows for the calculation of Helmholtz and Gibbs free energies and their temperature and pressure dependence and provide the corresponding computational tools. We employ non-equilibrium thermodynamics for evaluating…

Accurate phase diagram calculation from molecular dynamics requires systematic treatment and convergence of statistical averages. In this work we propose a Gaussian process regression based framework for reconstructing the free energy…

We present a method to accurately predict the Helmholtz harmonic free energies of molecular crystals in high-throughput settings. This is achieved by devising a computationally efficient framework that employs a Gaussian Process Regression…

Accurate prediction of thermodynamic properties requires an extremely accurate representation of the free energy surface. Requirements are twofold -- first, the inclusion of the relevant finite-temperature mechanisms, and second, a dense…

Phase diagrams serve as a highly informative tool for materials design, encapsulating information about the phases that a material can manifest under specific conditions. In this work, we develop a method in which Bayesian inference is…

We demonstrate an efficient and accurate, general-purpose first-principles blueprint for calculating anharmonic vibrational free energy and predicting structural phase transition temperatures of solids. Thermodynamic integration is…

Predictions of relative stabilities of (competing) molecular crystals are of great technological relevance, most notably for the pharmaceutical industry. However, they present a long-standing challenge for modeling, as often minuscule free…

Grain boundary (GB) properties greatly influence the mechanical, electrical, and thermal response of polycrystalline materials. Most computational studies of GB properties at finite temperatures use molecular dynamics (MD), which is…

The free energy and other thermodynamic properties of hexagonal-close-packed iron are calculated by direct {\em ab initio} methods over a wide range of pressures and temperatures relevant to the Earth's core. The {\em ab initio}…

Melting properties are critical for designing novel materials, especially for discovering high-performance, high-melting refractory materials. Experimental measurements of these properties are extremely challenging due to their high melting…

Atomic-scale phase-field modeling formulates the probability densities of atomic vibrations as Gaussian distributions and derives a free energy functional using variational Gaussian theory and interatomic potentials. This framework permits…

Phase diagrams are an invaluable tool for material synthesis and provide information on the phases of the material at any given thermodynamic condition. Conventional phase diagram generation involves experimentation to provide an initial…

We show how thermodynamic properties of molecular models can be computed over a large, multidimensional parameter space by combining multistate reweighting analysis with a linear basis function approach. This approach reduces the…

Point defects dictate the properties of many functional materials. The standard approach to modelling the thermodynamics of defects relies on a static description, where the change in Gibbs free energy is approximated by the internal…

Ensuring a satisfactory statistical convergence of anharmonic thermodynamic properties requires sampling of many atomic configurations, however the methods to obtain those necessarily produce correlated samples, thereby reducing the…

Reliable models of the thermodynamic properties of materials are critical for industrially relevant applications that require a good understanding of equilibrium phase diagrams, thermal and chemical transport, and microstructure evolution.…

Atomic structures and adatom geometries of surfaces encode information about the thermodynamics and kinetics of the processes that lead to their formation, and which can be captured by a generative physical model. Here we develop a workflow…

Free energy profiles serve as a fundamental bridge between microscopic atomic fluctuations and macroscopic thermodynamic observables. Estimating the free energy profile along a reaction coordinate, referred to as the potential of mean force…

The formally exact framework of equilibrium Density Functional Theory (DFT) is capable of simultaneously and consistently describing thermodynamic and structural properties of interacting many-body systems in arbitrary external potentials.…

Quantitative evaluations of the free energy of materials must take into account thermal and zero-point energy fluctuations. While these effects can easily be estimated within a harmonic approximation, corrections arising from the anharmonic…