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We present a calculation of the change of free energy of a solid surface upon bending of the solid. It is based on extracting the surface stress through a molecular dynamics simulation of a bent slab by using a generalized stress theorem…

Materials Science · Physics 2007-05-23 U. Tartaglino , D. Passerone , E. Tosatti , F. Di Tolla

Accurate calculations of solvation free energies remain a central challenge in molecular simulations, often requiring extensive sampling and numerous alchemical intermediates to ensure sufficient overlap between phase-space distributions of…

Statistical Mechanics · Physics 2026-04-02 Maximilian Schebek , Nikolas M. Froböse , Bettina G. Keller , Jutta Rogal

We analyse the finite-size corrections to the free energy of crystals with a fixed center of mass. When we explicitly correct for the leading ($\ln N/N$) corrections, the remaining free energy is found to depend linearly on 1/N.…

Statistical Mechanics · Physics 2009-10-31 J. M. Polson , E. Trizac , S. Pronk , D. Frenkel

This paper provides a concise description of the free energy principle, starting from a formulation of random dynamical systems in terms of a Langevin equation and ending with a Bayesian mechanics that can be read as a physics of sentience.…

Fluctuation relations allow for the computation of equilibrium properties, like free energy, from an ensemble of non-equilibrium dynamics simulations. Computing them for quantum systems, however, can be difficult, as performing dynamic…

Quantum Physics · Physics 2021-09-07 Lindsay Bassman , Katherine Klymko , Diyi Liu , Norman M. Tubman , Wibe A. de Jong

The free energy principle (FEP) from neuroscience provides a framework called active inference for the joint estimation and control of state space systems, subjected to colored noise. However, the active inference community has been…

Systems and Control · Electrical Eng. & Systems 2022-04-06 Ajith Anil Meera , Martijn Wisse

Free-energy differences between pairs of end-states can be estimated based on molecular dynamics (MD) simulations using standard pathway-dependent methods such as thermodynamic integration (TI), free-energy perturbation, or Bennett's…

The accurate but fast calculation of molecular excited states is still a very challenging topic. For many applications, detailed knowledge of the energy funnel in larger molecular aggregates is of key importance requiring highly accurate…

Chemical Physics · Physics 2024-01-12 Vivin Vinod , Sayan Maity , Peter Zaspel , Ulrich Kleinekathöfer

We propose a method, Temperature Integration, which allows an efficient calculation of free energy differences between two systems of interest, with the same degrees of freedom, which may have rough energy landscapes. The method is based on…

Statistical Mechanics · Physics 2015-06-12 Asaf Farhi , Guy Hed , Michael Bon , Nestor Caticha , Chi H Mak , Eytan Domany

Comparison of free energies between different phases and different compositions underlies the prediction of alloy phase diagrams. To allow direct comparison, consistent reference points for the energies or enthalpies are required, and the…

Materials Science · Physics 2021-05-19 Yang Huang , Michael Widom , Michael C. Gao

Computational modeling is an integral part of catalysis research. With it, new methodologies are being developed and implemented to improve the accuracy of simulations while reducing the computational cost. In particular, specific…

Materials Science · Physics 2024-08-28 Alexandre Boucher , Cameron Beevers , Bertrand Gauthier , Alberto Roldan

Calculating free energies is an important and notoriously difficult task for molecular simulations. The rapid increase in computational power has made it possible to probe increasingly complex systems, yet extracting accurate free energies…

Chemical Physics · Physics 2014-07-29 Viveca Lindahl , Jack Lidmar , Berk Hess

The Free Energy Principle (FEP) states that under suitable conditions of weak coupling, random dynamical systems with sufficient degrees of freedom will behave so as to minimize an upper bound, formalized as a variational free energy, on…

Quantum Physics · Physics 2022-07-21 Chris Fields , Karl Friston , James F. Glazebrook , Michael Levin

The free energy principle from neuroscience provides a brain-inspired perception scheme through a data-driven model learning algorithm called Dynamic Expectation Maximization (DEM). This paper aims at introducing an experimental design to…

Robotics · Computer Science 2021-09-27 Fred Bos , Ajith Anil Meera , Dennis Benders , Martijn Wisse

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…

Chemical Physics · Physics 2016-05-18 Levi N. Naden , Michael R. Shirts

Core-electron x-ray photoelectron spectroscopy is a powerful technique for studying the electronic structure and chemical composition of molecules, solids and surfaces. However, the interpretation of measured spectra and the assignment of…

Materials Science · Physics 2019-10-23 J. Matthias Kahk , Johannes Lischner

Retrosynthesis -- the process of identifying a set of reactants to synthesize a target molecule -- is of vital importance to material design and drug discovery. Existing machine learning approaches based on language models and graph neural…

Chemical Physics · Physics 2021-12-10 Ruoxi Sun , Hanjun Dai , Li Li , Steven Kearnes , Bo Dai

This report presents the application of polynomial regression for estimating free energy differences using thermodynamic integration. We employ linear regression to construct a polynomial that optimally fits the thermodynamic integration…

Computational Physics · Physics 2008-10-02 Conrad Shyu , F. Marty Ytreberg

We have considered a model of a small finite system with internal particles and surface degrees of freedom. All the main statistical distributions were explicitly obtained, on a pre thermodynamic limit basis. The concept of temperature or…

Statistical Mechanics · Physics 2025-08-11 D. M. Naplekov , V. V. Yanovsky

We propose an approach for computing the Gibbs free energy difference between phases of a material. The method is based on the determination of the average force acting on interfaces that separate the two phases of interest. This force,…

Statistical Mechanics · Physics 2015-10-26 Ulf R. Pedersen , Felix Hummel , Georg Kresse , Gerhard Kahl , Christoph Dellago