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

TL;DR

This paper introduces a new smoothing scheme that enables coupling all-electron full-potential DFT with grid-based continuum embedding models, enhancing simulation accuracy and interoperability for electrochemical and catalytic systems.

Contribution

A novel smoothing method that allows seamless integration of all-electron DFT with continuum embedding models on regular grids.

Findings

Successful coupling of Environ with FHI-aims

Benchmark simulations validate the smoothing scheme

Improved accuracy in electrostatic calculations

Abstract

Recent advances in continuum embedding models have enabled the incorporation of solvent and electrolyte effects into density functional theory (DFT) simulations of material surfaces, significantly benefiting electrochemistry, catalysis, and other applications. To extend the simulation of diverse systems and properties, the implementation of continuum embedding models into the Environ library adopts a modular programming paradigm, offering a flexible interface for communication with various DFT programs. The speed and scalability of the current implementation rely on a smooth definition of the key physical properties of the atomistic system, in particular of its electronic density. This has hindered the coupling of Environ with all-electron simulation packages, as the sharp electron density peaks near atomic nuclei are difficult to represent on regular grids. In this work, we introduce a novel smoothing scheme that transforms atom-centered electron densities into a regular grid representation while preserving the accuracy of electrostatic calculations. This approach enables a minimal and generic interface, facilitating seamless interoperability between Environ and all-electron DFT programs. We demonstrate this development through the coupling of Environ with the FHI-aims package and present benchmark simulations that validate the proposed method.