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We develop a method to fit high-temperature Gibbs free energy data for the development of interatomic potentials for atomic systems. The approach is based on Hamiltonian thermodynamic integration, enabling the identification of suitable…

Materials Science · Physics 2026-03-04 Liangrui Wei , Yang Sun

Various methods achieving importance sampling in ensembles of nonequilibrium trajectories enable to estimate free energy differences and, by maximum-likelihood post-processing, to reconstruct free energy landscapes. Here, based on Bayes…

Statistical Mechanics · Physics 2010-07-02 Manuel Athènes , Mihai-Cosmin Marinica

Based on a generative model (GM) and beliefs over hidden states, the free energy principle (FEP) enables an agent to sense and act by minimizing a free energy bound on Bayesian surprise. Inclusion of prior beliefs in the GM about desired…

Systems and Control · Electrical Eng. & Systems 2021-07-28 Thijs van de Laar , Ayça Özçelikkale , Henk Wymeersch

A simple, efficient, and accurate method is proposed to map multi-dimensional free energy landscapes. The method combines the temperature-accelerated molecular dynamics (TAMD) proposed in [Maragliano & Vanden-Eijnden, Chem. Phys. Lett. 426,…

Computational Physics · Physics 2009-11-13 Luca Maragliano , Eric Vanden-Eijnden

Taking advantage of the advances in generative deep learning, particularly normalizing flow, a framework, called Boltzmann Generator, has recently been proposed for the purpose of generating equilibrium atomic configurations from the…

Statistical Mechanics · Physics 2022-07-27 Rasool Ahmad , Wei Cai

Acylphosphatase (AcP) is a small protein with 98 amino acid residues that catalyzes the hydrolysis of carboxyl-phosphate bonds. AcP is a typical two-state protein with slow folding rate due to its relatively large contact order in the…

Soft Condensed Matter · Physics 2022-03-14 Xuening Ma , Hao Sun , Haiyan Hong , Zilong Guo , Huanhuan Su , Hu Chen

Metropolis simulations of all-atom models of peptides (i.e. small proteins) are considered. Inspired by the funnel picture of Bryngelson and Wolyness, a transformation of the updating probabilities of the dihedral angles is defined, which…

Statistical Mechanics · Physics 2009-11-10 Bernd A. Berg

Classical density-functional theory is the most direct approach to equilibrium structures and free energies of inhomogeneous liquids, but requires the construction of an approximate free-energy functional for each liquid of interest. We…

Soft Condensed Matter · Physics 2014-10-10 Ravishankar Sundararaman , Kendra Letchworth-Weaver , T A Arias

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…

Materials Science · Physics 2010-02-27 Pankaj A. Apte

Many materials processes and properties depend on the anisotropy of the energy of grain boundaries, i.e.~on the fact that this energy is a function of the five geometric degrees of freedom (DOF) of the interface. To access this parameter…

Materials Science · Physics 2023-07-26 Timo Schmalofski , Martin Kroll , Holger Dette , Rebecca Janisch

This article describes nonequilibrium techniques for the calculation of free energies of solids using molecular dynamics (MD) simulations. These methods provide an alternative to standard equilibrium thermodynamic integration methods and…

Materials Science · Physics 2022-01-13 Rodrigo Freitas , Mark Asta , Maurice de Koning

The free energetics of water density fluctuations in bulk water, at interfaces, and in hydrophobic confinement inform the hydration of hydrophobic solutes as well as their interactions and assembly. The characterization of such free…

Statistical Mechanics · Physics 2018-03-15 Erte Xi , Sean M. Marks , Suruchi Fialoke , Amish J. Patel

Machine-learned interatomic potentials (MLPs) provide near density functional theory (DFT) accuracy at reduced computational cost, but their reliability depends on representative training data and often deteriorates in transition-state…

Chemical Physics · Physics 2026-05-06 Ashique Lal , Rik S. Breebaart , Peter G. Bolhuis , Evert Jan Meijer

We developed a method for fitting machine-learning interatomic potentials with magnetic degrees of freedom, namely, magnetic Moment Tensor Potentials (mMTP). The main feature of our method consists in fitting mMTP to magnetic forces…

For planar and cubic Ising models, we examined two ways of approximation of a spectral density that describes a degeneracy of energy levels. We approximated the exponent of the spectral density by polynomials of even degrees and using our…

Disordered Systems and Neural Networks · Physics 2018-08-15 Leonid Litinskii , Boris Kryzhanovsky

This paper introduces an active learning approach to the fitting of machine learning interatomic potentials. Our approach is based on the D-optimality criterion for selecting atomic configurations on which the potential is fitted. It is…

Computational Physics · Physics 2017-09-19 Evgeny V. Podryabinkin , Alexander V. Shapeev

We introduce and analyze free energy landscapes defined by associating to any point inside the sphere a free energy calculated on a thin spherical band around it, using many orthogonal replicas. This allows us to reinterpret, rigorously…

Probability · Mathematics 2023-05-23 Eliran Subag

When studying high-dimensional dynamical systems such as macromolecules, quantum systems and polymers, a prime concern is the identification of the most probable states and their stationary probabilities or free energies. Often, these…

Data Analysis, Statistics and Probability · Physics 2013-01-01 Hao Wu , Frank Noé

The accurate prediction of protein-ligand binding affinities is crucial for drug discovery. Alchemical free energy calculations have become a popular tool for this purpose. However, the accuracy and reliability of these methods can vary…

Calculating free energy differences is a topic of substantial interest and has many applications including molecular docking and hydration, solvation, and binding free energies which is used in computational drug discovery. However, in…

Chemical Physics · Physics 2013-10-16 Asaf Farhi
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