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Fluctuation theorem and Onsager reciprocity relations.

D Andrieux1, P Gaspard

  • 1Center for Nonlinear Phenomena and Complex Systems, Universite Libre de Bruxelles, Code Postal 231, Campus Plaine, B-1050 Brussels, Belgium.

The Journal of Chemical Physics
|September 28, 2004
PubMed
Summary

This study derives Onsager reciprocity relations using a fluctuation theorem for nonequilibrium reactions. The theorem applies to systems in steady states, connecting macroscopic affinities and reaction constants.

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Area of Science:

  • Non-equilibrium thermodynamics
  • Chemical kinetics
  • Statistical mechanics

Background:

  • Onsager reciprocity relations are fundamental in thermodynamics.
  • Understanding nonequilibrium systems requires advanced theoretical frameworks.
  • The chemical master equation governs stochastic chemical reactions.

Purpose of the Study:

  • Derive Onsager and higher-order reciprocity relations.
  • Establish a fluctuation theorem for nonequilibrium reactions.
  • Connect macroscopic properties to microscopic dynamics.

Main Methods:

  • Utilizing the chemical master equation.
  • Applying a fluctuation theorem for generating functions of macroscopic fluxes.
  • Employing graph theory to identify macroscopic affinities.

Related Experiment Videos

  • Deriving Yamamoto-Zwanzig formulas for reaction constants.

    • Main Results:

    • Successfully derived Onsager and higher-order reciprocity relations.
    • Obtained a fluctuation theorem for nonequilibrium steady states.
    • Identified macroscopic affinities using graph theory.
    • Derived Yamamoto-Zwanzig formulas from the fluctuation theorem.

    Conclusions:

    • The fluctuation theorem provides a unified approach to nonequilibrium relations.
    • This work bridges statistical mechanics and macroscopic thermodynamics.
    • The findings offer new insights into the behavior of chemical systems far from equilibrium.