Adaptive molecular decomposition: large-scale quantum chemistry for liquids

Area of Science:

• Computational chemistry
• Materials science
• Physical chemistry

Background:

• Simulating liquid systems requires computationally efficient methods.
• Accurate modeling of electrolytes is crucial for battery development.
• Handling dynamic molecular configurations and reactions is challenging.

Purpose of the Study:

• To introduce a linear-scaling method for simulating liquids.
• To enable large-scale and long-time simulations of molecular systems.
• To accurately model chemical reactions in liquids.

Main Methods:

• Self-consistent charge non-orthogonal tight-binding.
• Many-body expansion adjusted dynamically to molecular configurations.
• Linear-scaling approach for computational efficiency.

Main Results:

• The method achieves linear scaling for liquid simulations.
• Excellent agreement with full tight-binding calculations for carbonate electrolytes.
• Successful simulation of liquids over large length and time scales.
• Correct handling of chemical reactions, including a correction for the Hellmann-Feynman theorem violation.

Conclusions:

• The developed method offers a computationally efficient and accurate approach for liquid simulations.
• It is particularly well-suited for studying electrolytes in lithium-ion batteries.
• The method's ability to handle reactions and large scales opens new possibilities in computational chemistry.