Equilibrium free-energy differences from nonequilibrium measurements: A master-equation approach
Physical review. E, Statistical physics, plasmas, fluids, and related interdisciplinary topicsPublished 1 November 1997Open access
Christopher Jarzynski
Citations1,341
Generate an AI Snapshot to get a quick, structured summary of this paper.
Study Snapshot
ObjectiveStudy objective
MethodsResearch methodology
PopulationPopulation studied
Sample sizeSample sizes
OutcomesStudy outcomes here
ResultsStudy results comes here
LimitationsResearch study limitations comes here
A concise AI-generated summary of the paper will appear here once you click Generate AI Snapshot.
Abstract
In has recently been shown that the Helmholtz free-energy difference between two equilibrium configurations of a system may be obtained from an ensemble of finite-time (nonequilibrium) measurements of the work performed in switching an external parameter of the system. Here this result is established, as an identity, within the master equation formalism. Examples are discussed and numerical illustrations provided.
Keywords
Physics and Astronomy
The Journal of Chemical PhysicsEquation of State Calculations by Fast Computing Machines
37,074 Citations1953N. Metropolis, Arianna W. Rosenbluth +3 more
Physical review. A, General physicsCanonical dynamics: Equilibrium phase-space distributions
23,341 Citations1985William G. Hoover
The dynamical steady-state probability density is found in an extended phase space with variables x, p/sub x/, V, epsilon-dot, and zeta, where the x are reduced distances and the two variables epsilus-dot andZeta act as thermodynamic friction coefficients.
The Journal of Chemical PhysicsA unified formulation of the constant temperature molecular dynamics methods
18,901 Citations1984Shūichi Nosé
Understanding Molecular Simulation: From Algorithms to Applications
6,407 Citations2001Daan Frenkel, Berend Smit
Journal of Computational PhysicsNonphysical sampling distributions in Monte Carlo free-energy estimation: Umbrella sampling
6,237 Citations1977G. M. Torrie, J. P. Valleau
Physical Review LettersNonequilibrium Equality for Free Energy Differences
5,351 Citations1997Christopher Jarzynski
The Journal of Chemical PhysicsStatistical Mechanics of Fluid Mixtures
3,481 Citations1935John G. Kirkwood
Journal of Computational PhysicsEfficient estimation of free energy differences from Monte Carlo data
2,778 Citations1976Charles H. Bennett
Near-optimal strategies are developed for estimating the free energy difference between two canonical ensembles, given a Metropolis-type Monte Carlo program for sampling each one, and their efficiency is never less or greater than that obtained by sampling only one ensemble.
Physics Today<i>Introduction to Modern Statistical Mechanics</i>
1,973 Citations1988David Chandler, J. K. Percus
NatureMolecular dynamics simulations in biology
1,120 Citations1990Martin Karplus, Gregory A. Petsko
Molecular dynamics is also being used to determine protein structures from NMR, to refine protein X-ray crystal structures faster from poorer starting models, and to calculate the free energy changes resulting from mutations in proteins.
Annual Review of Biophysics and Biophysical ChemistryFree Energy Via Molecular Simulation: Applications to Chemical and Biomolecular Systems
1,080 Citations1989David L. Beveridge, Frank M. DiCapua
Springer series in solid-state sciencesStatistical Physics II
959 Citations1985Ryogo Kubo, Morikazu Toda +1 more
Studies in modern thermodynamicsComputational Statistical Mechanics
608 Citations1991William G. Hoover
The Journal of Chemical PhysicsStatistical Mechanical Theory of Transport Processes. VII. The Coefficient of Thermal Conductivity of Monatomic Liquids
554 Citations1954Robert Zwanzig, John G. Kirkwood +2 more
Annual Review of Physical ChemistryComputational Alchemy
435 Citations1992Tjerk P. Straatsma, J. Andrew McCammon
The Journal of Chemical PhysicsFree energy of hydrophobic hydration: A molecular dynamics study of noble gases in water
297 Citations1986Tjerk P. Straatsma, Herman J. C. Berendsen +1 more
Physics Letters AKinetic moments method for the canonical ensemble distribution
245 Citations1996William G. Hoover, Brad Lee Holian
Physical Review LettersDirect dynamical calculation of entropy and free energy by adiabatic switching
233 Citations1990Masakatsu Watanabe, William P. Reinhardt
The results depend substantially on the form of the «switching» function, suggesting possible improvements in traditional thermodynamic switching processes and dynamical computation of differences in the Helmholtz free energy.
Journal of the American Chemical SocietyAn approach to the application of free energy perturbation methods using molecular dynamics: applications to the transformations of methanol .fwdarw. ethane, oxonium .fwdarw. ammonium, glycine .fwdarw. alanine, and alanine .fwdarw. phenylalanine in aqueous solution and to H3O+(H2O)3 .fwdarw. NH4+(H2O)3 in the gas phase
215 Citations1987U. Chandra Singh, Frank K. Brown +2 more
The Journal of Chemical PhysicsA finite-time variational method for determining optimal paths and obtaining bounds on free energy changes from computer simulations
66 Citations1993John E. Hunter, William P. Reinhardt +1 more
Journal of Statistical PhysicsThe goodness of ergodic adiabatic invariants
51 Citations1987Reggie Brown, Edward Ott +1 more
The Journal of Chemical PhysicsAbsolute entropy of simple point charge model water by adiabatic switching processes
29 Citations1994Li-Wen Tsao, Sheh‐Yi Sheu +1 more
Physical review. E, Statistical physics, plasmas, fluids, and related interdisciplinary topicsFree energy via thermostatted dynamic potential-energy changes
11 Citations1993Brad Lee Holian, Harald A. Posch +1 more
Three dynamical methods for computing canonical-ensemble Helmholtz free energies are discussed and compared for a thermostatted six-body harmonic chain and the one based on Kirkwood's coupling-parameter theory converges much more rapidly than do the two based on time-integrated heat transfer.