Designing explicit functionals for the charge density in terms of a potential

Abstract

One of the most powerful strategies to address properties of real many-body systems is to incorporate data obtained for models, for example, to use data of the homogeneous electron gas in order to build the Local Density Approximation for the Kohn-Sham exchange-correlation potential. In the present work, we examine to what extent we can use model data to design functionals directly for observables of materials. In particular, we study different approximations for the charge density of real inhomogeneous materials expressed as a simple, explicit functional of a given Kohn-Sham potential, using as central building block the Lindhard density-density response function of the homogeneous electron gas. Our increasingly realistic set of approximations includes a fully nearsighted expression equivalent to the Thomas-Fermi approximation, functional Taylor expansions, and different approximations to the Connector Theory developed in [Aouina \textit{et al.}, npj Computational Materials {\bf 11}, 242 (2025)]. In all cases, the charge density is obtained without ever solving the Kohn-Sham Schrödinger equation. Results for cubic helium, a prototypical strongly inhomogeneous material, as well as the covalent semiconductor silicon and metallic aluminum, systematically improve with higher levels of approximation. At the present stage, the results may be used for qualitative discussions or as optimized starting point for a self-consistent Kohn-Sham cycle. More generally, their quality indicates that this is a promising route to obtain functional expressions for observables that are relatively simple to calculate and to analyze.