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Coarse-graining models can be improved by accounting for many-body interactions. Adjusting three-body forces precisely controls the accuracy of coarse-grained simulations for systems like water.

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Area of Science:

  • Computational chemistry
  • Statistical mechanics
  • Materials science

Background:

  • Coarse-graining reduces system complexity by lowering degrees of freedom.
  • The accuracy of coarse-grained force fields depends on chosen basis functions.
  • Many-body interactions significantly influence pairwise potentials in coarse-grained models.

Purpose of the Study:

  • To investigate the impact of many-body extensions on coarse-grained force fields.
  • To develop a method for parametrizing coarse-grained potentials incorporating many-body effects.
  • To demonstrate control over simulation accuracy by tuning many-body interactions.

Main Methods:

  • Systematic reduction of degrees of freedom for coarse-graining.
  • Parametrization of two-body potentials followed by fitting three-body contributions.
  • Application to liquid water and liquid methanol systems.
  • Analysis of structural and thermodynamic properties.

Main Results:

  • Many-body extensions can alter two-body interactions, increasing attraction at short distances.
  • A method was proposed and illustrated to manage this interplay by sequential parametrization.
  • Three-body interactions are crucial for water's structure, while two-body interactions suffice for methanol's main features.
  • Varying three-body interaction strength allows control over model accuracy.

Conclusions:

  • Many-body effects are essential for accurate coarse-graining, particularly for systems like water.
  • The proposed parametrization strategy effectively incorporates many-body contributions.
  • Coarse-grained model accuracy can be systematically tuned via many-body terms.
  • Findings support developing basis sets that resolve many-body contributions by order.