Density-density functionals and effective potentials in many-body electronic structure calculations

TL;DR

This paper introduces new density-density functionals tailored to preserve specific properties of many-body ground states in non-interacting models, aiding the development of better trial wave functions for quantum Monte Carlo methods.

Contribution

It presents a theoretical framework for constructing density functionals that maintain certain ground state properties, enhancing electronic structure calculations.

Findings

The theory is extensible to various electronic structure methods.

It justifies the use of optimized empirical density functionals.

Validated with a near-analytic model.

Abstract

We demonstrate the existence of different density-density functionals designed to retain selected properties of the many-body ground state in a non-interacting solution starting from the standard density functional theory ground state. We focus on diffusion quantum Monte Carlo applications that require trial wave functions with optimal Fermion nodes. The theory is extensible and can be used to understand current practices in several electronic structure methods within a generalized density functional framework. The theory justifies and stimulates the search of optimal empirical density functionals and effective potentials for accurate calculations of the properties of real materials, but also cautions on the limits of their applicability. The concepts are tested and validated with a near-analytic model.