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Effective Two-Body Interactions.

Cameron Mackie1,2, Alexander Zech1, Martin Head-Gordon1,2

  • 1Department of Chemistry, University of California, Berkeley, California 94720, United States.

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|August 30, 2021
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Summary
This summary is machine-generated.

Cooperative effects in molecular interactions, crucial for condensed phases, can now be calculated more efficiently. This study presents a new method to quantify these complex many-body interactions, simplifying calculations for phenomena like hydrogen bonding and proton transfer.

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Area of Science:

  • Computational Chemistry
  • Quantum Chemistry
  • Molecular Interactions

Background:

  • Cooperative and nonadditive effects significantly influence pairwise noncovalent interactions in condensed phases.
  • These effects depend intricately on the molecular environment and arrangement.
  • Accurate quantification is essential for understanding chemical processes.

Purpose of the Study:

  • To develop general expressions for effective two-body interactions that account for many-body effects.
  • To simplify the calculation of cooperative phenomena in molecular systems.
  • To apply the developed methods to analyze cooperativity in water clusters and proton transfer.

Main Methods:

  • Formulation of general expressions for effective two-body interactions up to higher orders in the many-body expansion.
  • Development of a simplified approach requiring fewer individual calculations compared to traditional methods.
  • Application of energy decomposition analysis and cluster calculations for water and HCl-water systems.

Main Results:

  • A method is presented that simplifies calculations of many-body interactions, reducing computational cost.
  • For a model (H2O)8 cluster, electrical polarization was identified as the primary driver of cooperativity effects on hydrogen bonds.
  • Cooperative effects on proton transfer in an HCl + (H2O)4 cluster were characterized.

Conclusions:

  • The developed expressions provide an accurate and computationally efficient way to study cooperative effects.
  • This approach facilitates a deeper understanding of environmental influences on molecular interactions.
  • The findings have implications for modeling solvation, hydrogen bonding, and proton transfer processes.