Coupling all-electron full-potential density functional theory with grid-based continuum embeddings.

Area of Science:

• Computational chemistry
• Materials science
• Physical chemistry

Background:

• Continuum embedding models enhance density functional theory (DFT) simulations by including solvent and electrolyte effects.
• These models are crucial for applications in electrochemistry and catalysis.
• Current implementations face challenges with all-electron simulation packages due to difficulties in representing sharp electron densities on regular grids.

Purpose of the Study:

• To develop a novel smoothing scheme for representing atom-centered electron densities on regular grids.
• To enable seamless interoperability between the Environ library and all-electron DFT programs.
• To improve the speed and scalability of continuum embedding models in DFT simulations.

Main Methods:

• Introduction of a novel electron density smoothing scheme.
• Transformation of atom-centered densities to a regular grid representation.
• Coupling of the Environ library with the FHI-aims all-electron DFT package.

Main Results:

• The proposed smoothing scheme accurately represents electron densities on regular grids.
• Electrostatic calculations maintain accuracy after density transformation.
• Successful coupling of Environ with the FHI-aims package was demonstrated.
• Benchmark simulations validated the effectiveness of the new method.

Conclusions:

• The novel smoothing scheme overcomes limitations in coupling continuum embedding models with all-electron DFT programs.
• This development facilitates broader applications of DFT simulations in electrochemistry, catalysis, and materials science.
• The method provides a minimal and generic interface for enhanced computational chemistry research.