Modified Single Iteration Synchronous-Transit Approach to Bound Diffusion Barriers for Solid-State Reactions.

Area of Science:

• Materials Science
• Computational Chemistry
• Solid-State Physics

Background:

• Accurate prediction of material properties relies on understanding solid-state diffusion kinetics.
• Traditional methods for calculating diffusion barriers, like nudged elastic band (NEB), are computationally expensive.
• Accelerating materials screening requires more efficient computational approaches for diffusion analysis.

Purpose of the Study:

• To develop and validate a computationally efficient method for estimating solid-state diffusion barriers.
• To identify reliable upper and lower bounds for transition state (TS) energies.
• To enable high-throughput screening of materials for diffusion-controlled properties.

Main Methods:

• Proposed a modified single iteration synchronous-transit (MSIST) approach to identify TS energy bounds.
• Reduced computational demand by ∼70% compared to full NEB calculations, requiring only 30% of force evaluations.
• Validated MSIST by comparing its results with explicit NEB calculations across 53 cases.

Main Results:

• MSIST successfully bracketed NEB-calculated TS energies in all 53 comparative cases.
• Demonstrated MSIST's efficacy in analyzing Na+ diffusion in battery electrodes and oxygen vacancy diffusion in fuel cell components.
• Achieved average diffusion barrier ranges of 0.08 eV for Na+ diffusion and 0.33 eV in high-throughput screening of 97 materials.

Conclusions:

• MSIST offers a significant computational speedup for estimating diffusion barriers, enabling broader materials analysis.
• The method provides explicit error bounds, facilitating reliable data modeling and physical insight development.
• MSIST accelerates the discovery of materials with desirable diffusion properties for applications like batteries and fuel cells.