Toward Orbital-Free Density Functional Theory with Small Data Sets and Deep Learning

J Chem Theory Comput. 2022 Feb 8;18(2):1122-1128. doi: 10.1021/acs.jctc.1c00812. Epub 2022 Jan 7.

Abstract

We use voxel deep neural networks to predict energy densities and functional derivatives of electron kinetic energies for the Thomas-Fermi model and Kohn-Sham density functional theory calculations. We show that the ground-state electron density can be found via direct minimization for a graphene lattice without any projection scheme using a voxel deep neural network trained with the Thomas-Fermi model. Additionally, we predict the kinetic energy of a graphene lattice within chemical accuracy after training from only two Kohn-Sham density functional theory (DFT) calculations. We identify an important sampling issue inherent in Kohn-Sham DFT calculations and propose future work to rectify this problem. Furthermore, we demonstrate an alternative, functional derivative-free, Monte Carlo based orbital-free density functional theory algorithm to calculate an accurate two-electron density in a double inverted Gaussian potential with a machine-learned kinetic energy functional.