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Comprehensive classical analysis of partition function and some observables for weakly interacting polyatomic dimers.

Daniil N Chistikov1, Artem A Finenko1, Sergei E Lokshtanov1

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This study introduces a statistical method for calculating properties of dimers, like their partition function and equilibrium constant. The number of internal coordinates significantly impacts temperature dependence, crucial for understanding molecular interactions.

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Area of Science:

  • Physical Chemistry
  • Chemical Physics
  • Statistical Mechanics

Background:

  • Understanding the statistical mechanics of molecular dimers is essential for predicting their behavior in various conditions.
  • Previous methods often lacked a systematic approach for polyatomic dimers with weakly interacting rigid monomers.

Purpose of the Study:

  • To present a systematic classical statistical averaging procedure for calculating partition functions and equilibrium constants of polyatomic dimers.
  • To investigate the role of internal coordinates and kinematic coupling on the temperature dependence of the partition function.

Main Methods:

  • Derivation of kinetic energy for molecular pairs in a body-fixed frame.
  • Development of rigorous expressions for partition functions over specified phase space domains.
  • Application of statistical averaging for calculating observables.

Main Results:

  • The number of independent internal coordinates in a body-fixed frame is a critical factor determining the temperature dependence of the partition function.
  • A general approach was developed for calculating equilibrium constants of dimer formation and spectral moments of collision-induced absorption bands.
  • The method was demonstrated using a linear molecule-atom example.

Conclusions:

  • The presented statistical averaging procedure provides a robust framework for studying polyatomic dimers.
  • The findings highlight the importance of internal coordinate definition in statistical mechanics calculations for molecular systems.
  • This work facilitates accurate predictions of dimer properties and related spectroscopic phenomena.