Charge Distribution and Lithium Oxide Stability Modeled by Reactive Force Field.

Area of Science:

• Materials Science
• Computational Chemistry
• Electrochemistry

Background:

• Accurate modeling of lithium and its oxides is crucial for lithium battery design.
• Molecular dynamics is efficient for large structures but struggles with precise electron distribution.
• Existing methods for charge distribution approximation have limitations.

Purpose of the Study:

• To evaluate the impact of charge calculation methods on atomic charge reproduction.
• To optimize force field parameters for improved modeling of lithium and its oxides.
• To validate a novel reactive force field for lithium battery materials.

Main Methods:

• Utilized Kohn-Sham density functional theory approximated to the second order (ACKS2).
• Verified the effect of charge calculation methods on atomic charge reproduction.
• Optimized force field parameters for the ACKS2 method.
• Trained and validated a new ACKS2 reactive force field.

Main Results:

• The ACKS2 method shows improved charge distribution modeling compared to previous approaches.
• Optimized force field parameters alleviate perceived shortcomings of the ACKS2 method.
• The newly trained ACKS2 reactive force field accurately reproduces lithium and lithium-oxide crystal structures.
• The validated force field effectively models charge distribution in crystal slabs.

Conclusions:

• The developed ACKS2 reactive force field enhances the accuracy of modeling lithium and its oxides.
• This improved modeling capability is beneficial for the design and simulation of lithium batteries.
• The study demonstrates the potential of ACKS2 for reliable materials simulations.