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Solution, Solubility, and Solubility Equilibrium
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Relationship between Solvation Thermodynamics from IST and DFT Perspectives.

Ronald M Levy1, Di Cui1, Bin W Zhang1

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Inhomogeneous solvation theory (IST) and classical density functional theory (DFT) offer methods to calculate solution properties. DFT

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Area of Science:

  • Computational chemistry
  • Physical chemistry
  • Statistical mechanics

Background:

  • Inhomogeneous solvation theory (IST) and classical density functional theory (DFT) are frameworks for linking solution distribution functions to thermodynamic properties.
  • Both theories can be formulated using "end point" simulations of pure solvent and solution to determine solute chemical potential and local hydrating water properties.

Purpose of the Study:

  • To present the density functional theory (DFT) end point formulation for calculating solvation free energies.
  • To highlight the central role of the solute-solvent potential of mean force (PMF) in the DFT approach.
  • To demonstrate the application of DFT for analyzing solvation effects in molecular recognition.

Main Methods:

  • Formulating IST and DFT using two "end point" simulations.
  • Utilizing the solute-solvent potential of mean force (PMF) within the DFT framework.
  • Performing simulations of beta-cyclodextrin in water to analyze PMF components.

Main Results:

  • The DFT end point formulation provides local expressions for solute excess chemical potential.
  • The indirect part of the PMF in DFT corresponds to the lowest order truncation of IST.
  • Simulations of beta-cyclodextrin illustrate the behavior of PMF components during molecular binding.

Conclusions:

  • The DFT end point route offers an alternative to IST for studying solvation effects.
  • The solute-solvent PMF provides valuable insights into molecular recognition and conformational changes.
  • Understanding PMF components is crucial for analyzing host-guest interactions and molecular recognition processes.