Table 3 Comparison of classical MD and AIMD simulation parameters, HE cathodes, anodes, electrolyte applications, and limitations of HEM B/S

From: Toward high entropy material discovery for energy applications using computational and machine learning methods

Method

Parameters

Applications (HE Electrolytes)

Applications (cathodes and anodes)

Limitations

Classical MD

-System Size: 10⁵–10⁶ atoms

-Force Fields: Lennard-Jones, ReaxFF117, EAM224, MLFF225, COMPASS226, OPLS227.

-Time Scale: 1–100 ns, ~1 fs timestep

-Ensemble: NVT, NPT228.

-Software: LAMMPS229, GROMACS230.

-Config: Randomized HE atomic positions

-Box: Periodic, 10–100 nm

- Ion Transport: Ion conductivity, diffusion via MSD, migration pathways

- Solvation: RDFs for ion coordination, entropy-stabilized shells, anti-dendrite clustering

- Interface: SEI (solid-electrolyte interphase) thickness/composition, ion transfer rates, interfacial stress.

- Structural Dynamics: Lattice stability in HEOs, minimal volume change, phase transition suppression - Ion Diffusion: Ion kinetics, diffusion pathways

- Mechanical: Stress/strain during cycling, crack resistance

- No electronic structure modeling - Limited force field accuracy for HE systems

-No bond breaking/forming (except ReaxFF)

-Nanosecond/nanometer scale only

-Needs DFT/experimental validation

- Complex HE-FF development

AIMD

-System size: 102–103 atoms

-Method: DFT (PBE231, HSE06232), PAW pseudopotentials233.

-Time Scale: 10–100 ps, ~0.5–1 fs timestep

-Ensemble: NVT

-Software: VASP234, Quantum ESPRESSO235.

-Config: DFT-optimized HE structures

-Box: Periodic, 1–10 nm

-Settings: k-points, 400–600 eV cutoff

- Electronic Structure: Ion-solvent charge transfer, DOS for coordination, polarization effects - Reactions: SEI formation pathways, bond breaking/forming, complex stability

- Ion Dynamics: Diffusion barriers, vibrational spectra

- Redox Properties: DOS for voltage stability, redox potentials, entropy effects - Diffusion: Ion migration energies, transition state analysis

- Local Structure: Short-range order, defect energies

- Electronic effects: Band structure changes, conductivity in HEAs

- Stability: Surface reaction energies, degradation pathways

- Dynamics: Ion adsorption kinetics, surface diffusion

-High computational cost - small system size (102–103 atoms)

-Short timescale (10–100 ps)

-DFT functional accuracy issues

-Not scalable for high-throughput -Complex setup for HE systems

-Convergence issues in disordered HE materials

Back to article page