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Memory Effects Explain the Fractional Viscosity Dependence of Rates Associated with Internal Friction: Simple Models

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Biophysical processes deviate from Kramers

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Area of Science:

  • Biophysics
  • Chemical Physics
  • Computational Chemistry

Background:

  • Barrier-crossing rates in biophysical processes often deviate from Kramers' theory.
  • Deviations are frequently attributed to internal friction, but solvent effects can also play a role.
  • Previous work highlighted memory-dependent friction from nonequilibrium solvation as a cause for misinterpretation.

Purpose of the Study:

  • To investigate the origin of internal friction in biomolecular systems.
  • To develop a model that captures memory effects without explicit solvent.
  • To propose a microscopic measure for internal friction in biological contexts.

Main Methods:

  • Introduction of a simple diatom model to study internal memory effects.
  • Analysis of the coupling between reaction coordinate motion and orthogonal degrees of freedom.
  • Application of Grote-Hynes theory for microscopic friction measurement.
  • Demonstration using butane to study coupling strength effects.

Main Results:

  • A simple diatom model without explicit solvent exhibits internal memory effects.
  • Coupling to orthogonal degrees of freedom leads to fractional viscosity dependence.
  • This fractional dependence mimics internal friction, deviating from Kramers' theory.
  • Grote-Hynes theory provides a microscopic measure of this emergent friction.

Conclusions:

  • Internal memory effects, not just explicit solvent, can cause deviations from Kramers' theory.
  • The diatom model effectively mimics internal friction observed in biomolecular conformational changes.
  • This framework aids in understanding biological internal friction through coupling effects.