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Stochastic level-set variational implicit-solvent approach to solute-solvent interfacial fluctuations.

Shenggao Zhou1, Hui Sun2, Li-Tien Cheng2

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This study introduces a new computational method to include interfacial fluctuations in implicit-solvent models, improving biomolecular simulations. The approach captures dewetting transitions and reveals how fluctuations impact solvation free energies.

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Area of Science:

  • Computational chemistry and biophysics
  • Molecular modeling and simulation
  • Statistical mechanics

Background:

  • The variational implicit-solvent model (VISM) successfully estimates biomolecular solvation free energies and hydration states.
  • VISM's level-set minimization predicts equilibrium conformations but often relies on initial guesses and neglects interfacial fluctuations.
  • Interfacial fluctuations are critical for biomolecular conformational changes and binding processes.

Purpose of the Study:

  • To develop a theoretical framework and numerical methods to incorporate solute-solvent interfacial fluctuations into the VISM.
  • To investigate the impact of these fluctuations on biomolecular solvation and conformational dynamics.
  • To study dewetting transitions in hydrophobic systems using the enhanced VISM.

Main Methods:

  • Developed a Langevin geometrical flow theory to model interfacial fluctuations.
  • Implemented a stochastic level-set method for numerical simulations, ensuring representation independence.
  • Applied the computational method to systems of two hydrophobic plates and a cucurbit[7]uril host molecule.

Main Results:

  • The enhanced VISM successfully captures dewetting transitions and systems jumping out of free-energy local minima.
  • For two hydrophobic plates, interfacial fluctuation wavelength significantly influences dewetting.
  • The dewetting energy barrier scales quadratically with inter-plate distance, consistent with molecular dynamics simulations.

Conclusions:

  • This work represents a significant step towards including interfacial fluctuations in implicit-solvent models.
  • The developed method provides a robust approach to study the impact of fluctuations on biomolecular solvation.
  • The findings offer new insights into hydrophobic effects and conformational changes in biomolecular systems.