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We present the energetic aspect of open systems which may exchange particles with their environments. Our attention shall be paid to the scale that the motion of the particles is described by the classical Langevin dynamics. Along a…

Statistical Mechanics · Physics 2009-10-31 Tatsuo Shibata , Ken Sekimoto

The process of deriving an interatomic potentials represents an attempt to integrate out the electronic degrees of freedom from the full quantum description of a condensed matter system. In practice it is the derivatives of the interatomic…

Materials Science · Physics 2016-06-23 G. J. Ackland

We present a Monte Carlo simulation technique by which the free energy of disordered systems can be computed directly. It is based on thermodynamic integration. The central idea is to construct an analytically solvable reference system from…

Statistical Mechanics · Physics 2015-05-14 Tanja Schilling , Friederike Schmid

The calculation of caloric properties such as heat capacity, Joule-Thomson coefficients and the speed of sound by classical force-field-based molecular simulation methodology has received scant attention in the literature, particularly for…

Chemical Physics · Physics 2019-03-15 William R. Smith , Jan Jirsák , Ivo Nezbeda , Weikai Qi

Free energies play a central role in characterising the behaviour of chemical systems and are among the most important quantities that can be calculated by molecular dynamics simulations. Solvation free energies in various organic solvents,…

Chemical Physics · Physics 2026-02-11 J. Harry Moore , Daniel J. Cole , Gabor Csanyi

We study whether the stationary state of two bulk-driven systems slowly exchanging particles can be described by the equality of suitably defined nonequilibrium chemical potentials. Our main result is that in a weak contact limit, chemical…

Statistical Mechanics · Physics 2018-08-29 Jules Guioth , Éric Bertin

We introduce a simulation technique to compute the free energy difference between two hydrate structures of different stoichiometry connected to a reservoir of gas molecules at a prescribed pressure. The method permits the determination of…

Chemical Physics · Physics 2026-04-16 Olivia S. Moro , Nigel B. Wilding , Vincent Ballenegger

We derive a new formulation to calculate the excess chemical potential of a fraction of $N_1$ particles interacting with $N_2$ particles of a different species. The excess chemical potential is calculated numerically from first principles…

Astrophysics · Physics 2008-11-26 Christophe Winisdoerffer , Gilles Chabrier , Gilles Zérah

The hydration or binding free energy of a drug-like molecule is a key data for early stage drug discovery. Hundreds of thousands of evaluations are needed, which rules out the exhaustive use of atomistic simulations and free energy methods.…

Chemical Physics · Physics 2018-06-11 Sohvi Luukkonen , Luc Belloni , Daniel Borgis , Maximilien Levesque

Three-parametric Lenard-Jones and Morse interatomic potentials are the simplest ones, which that can be used to obtain thermophysical properties of the liquid and solid substances. Upon adjusting the model parameters to real substance…

Materials Science · Physics 2022-09-29 A. A. Likhachev , Yu. N. Koval , T. G. Sych , V. A. Tatarenko

Molecular dynamics simulations at a constant electric potential are an essential tool to study electrochemical processes, providing microscopic information on the structural, thermodynamic, and dynamical properties. Despite the numerous…

We present a method for computing free-energy differences using thermodynamic integration with a neural network potential that interpolates between two target Hamiltonians. The interpolation is defined at the sample distribution level, and…

Statistical Mechanics · Physics 2025-03-26 Bálint Máté , François Fleuret , Tristan Bereau

We propose a new method to obtain kinetic properties of infrequent events from molecular dynamics simulation. The procedure employs a recently introduced variational approach [Valsson and Parrinello, Phys. Rev. Lett. 113, 090601 (2014)] to…

Statistical Mechanics · Physics 2015-08-19 James McCarty , Omar Valsson , Pratyush Tiwary , Michele Parrinello

The definition of the fundamental quantity, the chemical potential, is badly confused in the literature: there are at least three distinct definitions in various books and papers. While they all give the same result in the thermodynamic…

Statistical Mechanics · Physics 2007-05-23 T. A. Kaplan

Studying chemical reactions, particularly in the gas phase, relies heavily on computing scattering matrix elements. These elements are essential for characterizing molecular reactions and accurately determining reaction probabilities.…

Quantum Physics · Physics 2024-04-24 Sumit Suresh Kale , Sabre Kais

Controlling polymorphism in molecular crystals is crucial in the pharmaceutical, dye, and pesticide industries. However, its theoretical description is extremely challenging, due to the associated long timescales ($ > 1 \, \mu s$). We…

Chemical Physics · Physics 2023-02-09 Oren Elishav , Roy Podgaetsky , Olga Meikler , Barak Hirshberg

We propose a method for identifying holographic chemical potentials of conserved charges. The guiding principle is the consistency of the identification with the thermodynamic relations and the Legendre transformation. We consider the…

High Energy Physics - Theory · Physics 2008-12-30 Shin Nakamura

Computing vibrational free energies ($F_{vib}$) and entropies ($S_{vib}$) has posed a long standing challenge to the high-throughput ab initio investigation of finite temperature properties of solids. Here we use machine-learning techniques…

Materials Science · Physics 2017-03-08 Fleur Legrain , Jesús Carrete , Ambroise van Roekeghem , Stefano Curtarolo , Natalio Mingo

Calculating relative free energies is a topic of substantial interest and has many applications including solvation and binding free energies, which are used in computational drug discovery. However, there remain the challenges of accuracy,…

Chemical Physics · Physics 2016-09-28 Asaf Farhi , Bipin Singh

We demonstrate that the machine learning of density functionals allows one to determine simultaneously the equilibrium chemical potential across simulation datasets of inhomogeneous classical fluids. Minimization of a loss function based on…

Soft Condensed Matter · Physics 2026-02-11 Florian Sammüller , Matthias Schmidt