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Related Experiment Video

Updated: May 12, 2026

An Analog Macroscopic Technique for Studying Molecular Hydrodynamic Processes in Dense Gases and Liquids

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Published on: December 4, 2017

Reconstructing equilibrium entropy and enthalpy profiles from non-equilibrium pulling.

Daun Jeong¹, Ioan Andricioaei

¹Department of Chemistry, University of California, Irvine, California 92697, USA.

The Journal of Chemical Physics

|March 29, 2013

Summary

This study presents novel methods to decompose free energy profiles into entropy and energy components using non-equilibrium trajectories. These findings enable accurate analysis of biomolecular systems without repeated experiments.

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Area of Science:

Statistical Mechanics
Computational Biophysics
Physical Chemistry

Background:

The Jarzynski identity allows calculating equilibrium free energy from non-equilibrium work measurements.
Decomposing free energy into entropy and energy components is crucial for understanding molecular processes.

Purpose of the Study:

To derive analytical expressions for temperature derivatives of free energy profiles.
To develop methods for decomposing free energy into equilibrium entropy and internal energy profiles from non-equilibrium data.
To provide a single-temperature decomposition method, avoiding repeated measurements.

Main Methods:

Utilizing Wiener stochastic path integrals with temperature-dependent weights for Langevin trajectories.
Deriving exact formulae for temperature derivatives of free energy.
Applying three distinct analytical expressions: generalized weighted histogram analysis, quasi-harmonic spring limit, and Feynman-Kac formula.

Main Results:

Exact formulae for temperature derivatives of free energy profiles were derived.
Analytical expressions for entropy-energy decomposition from non-equilibrium pulling were obtained.
The methods were validated using Langevin simulations of a 2D model for biomolecular conformational changes.

Conclusions:

The developed methods enable accurate decomposition of free energy profiles into entropy and energy components.
This approach simplifies analysis by requiring trajectories at a single temperature.
The study suggests connections to single-molecule experiments for probing necessary functionals.