From localized orbitals to material properties: building classical force fields for nonmetallic condensed matter...

Area of Science:

• Computational chemistry
• Materials science
• Condensed matter physics

Background:

• The accuracy of atomic-scale simulations relies heavily on the quality of force fields.
• Developing predictive force fields from first principles remains a significant challenge in computational materials science.

Purpose of the Study:

• To present a novel method for generating reliable and predictive force fields from ab initio simulations.
• To demonstrate the capability of using maximally localized Wannier orbitals (WO) for deriving interatomic interactions.

Main Methods:

• Employing ab initio simulations in the condensed phase.
• Utilizing maximally localized Wannier orbitals (WO) to derive individual interaction terms (electrostatic, exchange repulsion, dispersion, induction).
• Applying the method to condensed-phase systems like molten salts and liquid water.

Main Results:

• Successfully generated predictive force fields with excellent accuracy for tested materials.
• Demonstrated that localized WOs effectively capture electrostatic, exchange repulsion, dispersion, and induction interactions.
• Validated the approach for both ionic liquids and molecular liquids.

Conclusions:

• The proposed method offers a robust route to high-fidelity force fields from electronic structure calculations.
• Maximally localized Wannier orbitals serve as a crucial bridge connecting electronic structure details to macroscopic material properties.
• The approach supports the application of chemical concepts, like Lewis pairs, in condensed-phase simulations.