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This study derives an analytical excess entropy scaling relation for coarse-grained (CG) systems. It uses effective hard sphere models to accurately predict CG system dynamics and diffusion coefficients.

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Area of Science:

  • Physical Chemistry
  • Computational Chemistry
  • Statistical Mechanics

Background:

  • Excess entropy scaling is a universal principle observed in both fine-grained and coarse-grained (CG) systems.
  • Previous studies demonstrated this universality but lacked a precise analytical framework due to semi-empirical limitations.

Purpose of the Study:

  • To derive an analytical excess entropy scaling relation for bottom-up CG systems.
  • To develop a method for accurately predicting the dynamics and diffusion of molecular liquids using hard sphere reference fluids.

Main Methods:

  • Constructed effective hard sphere systems at single-site CG resolution to match CG system dynamics.
  • Employed a "fluctuation matching" approach to equate density fluctuations (dimensionless compressibility) between CG and hard sphere systems.
  • Utilized Enskog theory to derive hard sphere diffusion coefficients and bridge CG dynamics with excess entropy.

Main Results:

  • Developed an analytical excess entropy scaling relation applicable to bottom-up CG systems.
  • Demonstrated that effective hard sphere systems can accurately replicate the dynamical properties of CG systems.
  • Enabled rough estimation of CG diffusion coefficients using equations of state and accurate prediction of accelerated CG dynamics.

Conclusions:

  • The derived analytical relation provides a more rigorous framework for assessing excess entropy scaling.
  • The proposed method allows for accurate prediction of CG dynamics without extensive simulations.
  • This work advances the understanding of accelerated CG dynamics in molecular fluids.