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Molecular dynamics is a powerful tool for studying the thermodynamics and kinetics of complex molecular events. However, these simulations can rarely sample the required time scales in practice. Transition path sampling overcomes this…

Chemical Physics · Physics 2023-07-31 Gianmarco Lazzeri , Hendrik Jung , Peter G. Bolhuis , Roberto Covino

In this work, I propose a statistical mechanical framework, for the evaluation of the free energy in molecular systems, by "deleting" all the molecules in a "single" step. The approach can be considered as the statistical mechanics…

Statistical Mechanics · Physics 2011-08-16 Georgios C. Boulougouris

In this paper we study computationally feasible bounds for relative free energies between two many-particle systems. Specifically, we consider systems out of equilibrium that do not necessarily satisfy a fluctuation-dissipation relation,…

Statistical Mechanics · Physics 2024-03-19 Luigi Delle Site , Carsten Hartmann

We study a class of non-equilibrium quasi-stationary states for a Markov system interacting with two different thermal baths. We show that the work done under a slow, external change of parameters admits a potential, i.e., the free energy.…

Statistical Mechanics · Physics 2017-05-23 A. E. Allahverdyan , N. H. Martirosyan

The Gibbs free energy is the fundamental thermodynamic potential underlying the relative stability of different states of matter under constant-pressure conditions. However, computing this quantity from atomic-scale simulations is far from…

Materials Science · Physics 2018-02-14 Bingqing Cheng , Michele Ceriotti

Jarzynski's identity for the free energy difference between two equilibrium states can be viewed as a special case of a more general procedure based on phase space mappings. Solving a system's equation of motion by approximate means…

Statistical Mechanics · Physics 2009-11-11 Wolfgang Lechner , Harald Oberhofer , Christoph Dellago , Phillip L. Geissler

Recent experiments indicate that electromagnetic hysteresis behavior can be exhibited at the molecular level.A MD simulation using 2-body potentials and switches to form and break bonds is implemented to determine whether chemical reaction…

Computational Physics · Physics 2007-05-23 Christopher G. Jesudason

Phase diagrams (PDs) illustrate the relative stability of competing phases under varying conditions, serving as critical tools for synthesizing complex materials. Reliable phase diagrams rely on precise free energy calculations, which are…

Materials Science · Physics 2026-02-09 Feng Zhang , Zhuo Ye , Maxim Moraru , Ying Wai Li , Weiyi Xia , Yongxin Yao , Cai-Zhuang Wang

A Hamiltonian-based model of many harmonically interacting massive particles that are subject to linear friction and coupled to heat baths at different temperatures is used to study the dynamic approach to equilibrium and non-equilibrium…

Statistical Mechanics · Physics 2020-09-17 Roland R. Netz

This paper introduces a method for computing the Helmholtz free energy using the flow matching technique. Unlike previous work that utilized flow-based models for variational free energy calculations, this method provides bounds for free…

Computational Physics · Physics 2025-01-03 Lu Zhao , Lei Wang

We present a history-dependent Monte Carlo scheme for the efficient calculation of the free-energy of quantum systems, inspired by the Wang-Landau sampling and metadynamics method. When embedded in a path integral formulation, it is of…

Statistical Mechanics · Physics 2009-04-08 Yanier Crespo , Alessandro Laio , Giuseppe E. Santoro , Erio Tosatti

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 solid-liquid interface free energy \gamma sl 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…

Materials Science · Physics 2010-05-20 Stefano Angioletti-Uberti , Michele Ceriotti , Mike W. Finnis , Peter D. Lee

Using a recently developed technique to estimate the equilibrium free energy of glassy materials, we explore if equilibrium simulation methods can be used to estimate the solubility of amorphous solids. As an illustration, we compute the…

Statistical Mechanics · Physics 2021-04-07 H. A. Vinutha , Daan Frenkel

The computation of free energy differences through an exponential weighting of out of equilibrium paths (known as the Jarzynski equality) is often used for transitions between states described by an external parameter $\lambda$ in the…

Statistical Mechanics · Physics 2015-06-25 Tony Lelievre , Mathias Rousset , Gabriel Stoltz

Free energy perturbation (FEP) is frequently used to evaluate the free energy change of a biological process, e.g. the drug binding free energy or the ligand solvation free energy. Due to the sampling inefficiency, FEP is often employed…

Chemical Physics · Physics 2017-01-31 Ying-Chih Chiang , Frank Otto

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

In this study, we carried out equilibrium molecular dynamics (EMD) simulations of the liquid-liquid interface between two different Lennard-Jones components with varying miscibility, where we examined the relation between the interfacial…

Soft Condensed Matter · Physics 2025-12-29 Rei Ogawa , Hiroki Kusudo , Takeshi Omori , Edward R. Smith , Laurent Joly , Samy Merabia , Yasutaka Yamaguchi

The shift in chemical equilibria due to isotope substitution is often exploited to gain insight into a wide variety of chemical and physical processes. It is a purely quantum mechanical effect, which can be computed exactly using…

Statistical Mechanics · Physics 2014-07-04 Michele Ceriotti , Thomas E. Markland

A central endeavor of thermodynamics is the measurement of free energy changes. Regrettably, although we can measure the free energy of a system in thermodynamic equilibrium, typically all we can say about the free energy of a…

Statistical Mechanics · Physics 2012-04-10 David A. Sivak , Gavin E. Crooks