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Including atomic polarisability in molecular dynamics simulations enhances ionic liquid fluidity and reduces structural complexity. This charge flexibility acts similarly to adding a co-solvent, improving simulation accuracy.

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Area of Science:

  • Computational Chemistry
  • Materials Science
  • Physical Chemistry

Background:

  • Classical Molecular Dynamics (MD) simulations often use fixed point charges for electrostatic interactions.
  • Atomic polarisability, or charge flexibility, can more accurately model these interactions.
  • Existing MD models like Drude oscillators and induced point-dipoles offer ways to incorporate polarisability.

Purpose of the Study:

  • To systematically compare Drude oscillators and induced point-dipoles for modelling atomic polarisability in MD simulations.
  • To investigate the impact of polarisable hydrogen atoms on simulation results.
  • To quantify the effect of varying polarisability strength on ionic liquid properties.

Main Methods:

  • Comparison of Drude oscillator and induced point-dipole models using CHARMM and AMBER software.
  • Systematic increment of atomic polarisability strength in 10% steps.
  • Analysis of ionic liquid 1-ethyl-3-methylimidazolium triflate (EMIM(⊕)CF3SO) structure and dynamics.

Main Results:

  • Increased atomic polarisability generally leads to enhanced fluidity in the ionic liquid.
  • Charge flexibility results in less pronounced structural ordering within the ionic liquid.
  • The inclusion of polarisability significantly influences the simulated dynamics and structure.

Conclusions:

  • Atomic polarisability is crucial for accurately simulating ionic liquid behavior.
  • Incorporating polarisability can mimic the effects of adding a co-solvent, acting as an 'inner solvent'.
  • The study provides a framework for parameterizing polarisable models in MD simulations.