Neural network distillation of orbital dependent density functional theory

TL;DR

This paper introduces a neural network framework to simplify complex density functionals in DFT, enabling efficient computation of potentials and derivatives, with high transferability across molecular systems.

Contribution

It presents a novel neural network approach to model orbital-dependent density functionals as global density approximations, improving computational efficiency and transferability.

Findings

Successfully eliminated orbital dependencies from kinetic energy density

Achieved high transferability to various molecular systems

Enabled automatic differentiation for nonlinear response functions

Abstract

Density functional theory (DFT) offers a desirable balance between quantitative accuracy and computational efficiency in practical many-electron calculations. Its central component, the exchange-correlation energy functional, has been approximated with increasing levels of complexity ranging from strictly local approximations to nonlocal and orbital-dependent expressions with many tuned parameters. In this paper, we formulate a general way of rewriting complex density functionals using deep neural networks in a way that allows for simplified computation of Kohn-Sham potentials as well as higher functional derivatives through automatic differentiation, enabling access to highly nonlinear response functions and forces. These goals are achieved by using a recently developed class of robust neural network models capable of modeling functionals, as opposed to functions, with explicitly enforced spatial symmetries. Functionals treated in this way are then called global density approximations and can be seamlessly integrated with existing DFT workflows. Tests are performed for a dataset featuring a large variety of molecular structures and popular meta-generalized gradient approximation density functionals, where we successfully eliminate orbital dependencies coming from the kinetic energy density, and discover a high degree of transferability to a variety of physical systems. The presented framework is general and could be extended to more complex orbital and energy dependent functionals as well as refined with specialized datasets.