PMID: 22587237May 17, 2012Paper

Near-equilibrium measurements of nonequilibrium free energy

Physical Review Letters
David A Sivak, Gavin E Crooks

Abstract

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 nonequilibrium ensemble is that it is larger than that of the same system at equilibrium. Herein, we derive a formally exact expression for the probability distribution of a driven system, which involves path ensemble averages of the work over trajectories of the time-reversed system. From this we find a simple near-equilibrium approximation for the free energy in terms of an excess mean time-reversed work, which can be experimentally measured on real systems. With analysis and computer simulation, we demonstrate the accuracy of our approximations for several simple models.

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Citations

Sep 4, 2012·The Journal of Chemical Physics·M Scott Shell
Nov 10, 2014·The Journal of Chemical Physics·Folarin LatinwoCharles M Schroeder
Feb 24, 2016·The Journal of Physical Chemistry. B·Mazen AhmadThomas Lengauer
May 15, 2015·PloS One·Hailey R BureauRigoberto Hernandez
Nov 5, 2015·Nature Nanotechnology·Jeremy L England
Sep 26, 2012·Physical Review Letters·David A Sivak, Gavin E Crooks
Dec 12, 2012·Physical Review. E, Statistical, Nonlinear, and Soft Matter Physics·Patrick R ZulkowskiMichael R DeWeese
Sep 26, 2012·Physical Review Letters·Susanne StillGavin E Crooks
Dec 15, 2016·Physical Review. E·David A Sivak, Gavin E Crooks
Jan 20, 2018·Physical Review. E·Geng LiZ C Tu
Jul 18, 2018·Physical Review. E·Marcelo M de OliveiraCarlos E Fiore
Feb 20, 2019·Physical Review. E·Joseph N E LuceroDavid A Sivak
Aug 31, 2016·Physical Review. E·Sebastian DeffnerWojciech H Zurek
Feb 6, 2020·Proceedings of the National Academy of Sciences of the United States of America·Samuel J Bryant, Benjamin B Machta
Apr 15, 2016·Physical Review. E·Gabriel T Landi, Dragi Karevski
Aug 28, 2020·Physical Review Letters·Akira SonePaola Cappellaro
Oct 30, 2014·Physical Review. E, Statistical, Nonlinear, and Soft Matter Physics·Patrick R Zulkowski, Michael R DeWeese
Dec 17, 2018·The Journal of Chemical Physics·Owen LeddyAaron R Dinner
Jan 9, 2017·The Journal of Chemical Physics·Mazen AhmadThomas Lengauer
Mar 19, 2013·Physical Review. E, Statistical, Nonlinear, and Soft Matter Physics·Naoko Nakagawa, Shin-ichi Sasa
Nov 18, 2015·Journal of Chemical Theory and Computation·Mazen AhmadOlga V Kalinina
Aug 15, 2019·Chemical Reviews·Aidan I Brown, David A Sivak

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