Correcting Delocalization Error in Materials with Localized Orbitals and Linear-Response Screening

TL;DR

This paper introduces lrLOSC, a method to correct delocalization errors in DFT, significantly improving the accuracy of band gap predictions and molecular properties across various materials.

Contribution

The paper presents lrLOSC, a novel correction technique for delocalization errors in DFT that enhances accuracy for materials and molecular properties.

Findings

Predicted fundamental gaps within 0.22 eV for eleven materials.

Improved molecular property predictions with parallel implementation.

Offers a nonzero total energy correction for materials.

Abstract

Delocalization error prevents density functional theory (DFT) from reaching its full potential, causing problems like systematically underestimated band gaps and misaligned energy levels at interfaces. We introduce lrLOSC to correct delocalization error in materials over a wide range of band gaps. We predict eleven materials' fundamental gaps to within 0.22 eV, while offering a nonzero total energy correction; molecular properties are improved with a parallel implementation of the same theory [J. Phys. Chem. Lett. 16, 2492 (2025)]. lrLOSC is an essential step toward modeling molecules, materials, and their interfaces within the same DFT framework.