Simultaneous estimation of free energies and rates using forward flux sampling and mean first passage times

In this work, a method is proposed to simultaneously compute the transition rate constant and the free energy profile of a rare event along an order parameter connecting two well-defined regions of phase space. The method employs a forward flux sampling technique in combination with a mean first pas...

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Published in:The Journal of chemical physics 2015-12, Vol.143 (24), p.244113-244113
Main Authors: Thapar, Vikram, Escobedo, Fernando A
Format: Article
Language:English
Subjects:
Free energy
Ising model
Markov analysis
Markov chains
Nucleation
Order parameters
Physics
Potential energy
Sampling
Solid phases
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description In this work, a method is proposed to simultaneously compute the transition rate constant and the free energy profile of a rare event along an order parameter connecting two well-defined regions of phase space. The method employs a forward flux sampling technique in combination with a mean first passage time approach to estimate the steady state probability and mean first passage times. These quantities are fitted to a Markovian model that allows the estimation of the free energy along the chosen order parameter. The proposed technique is first validated with two test systems (an Ising model and a model potential energy surface) and then used to study the solid-phase homogeneous nucleation of selected polyhedral particles.
doi_str_mv 10.1063/1.4938248
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source American Institute of Physics (AIP) Publications; American Institute of Physics:Jisc Collections:Transitional Journals Agreement 2021-23 (Reading list)
subjects Free energy
Ising model
Markov analysis
Markov chains
Nucleation
Order parameters
Physics
Potential energy
Sampling
Solid phases
title Simultaneous estimation of free energies and rates using forward flux sampling and mean first passage times
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