Self-Consistent Calculation of the Localized Orbital Scaling Correction for Correct Electron Densities and Energy-Level Alignments in Density Functional Theory.

Journal Article (Journal Article)

The recently developed localized orbital scaling correction (LOSC) method shows the ability to systematically and size-consistently reduce the delocalization error existing in conventional density functional approximations (DFAs). However, the application of LOSC to DFAs was mainly through a post self-consistent field (SCF) manner, and few results from applying LOSC to DFAs in an SCF manner have been reported. The reason is that the originally proposed SCF approach to SCF-LOSC calculation uses an approximate Hamiltonian and encounters convergence problems easily in practice. In this work, we develop a new SCF approach with a correct Hamiltonian and achieve reliable SCF-LOSC calculations. We demonstrate the capability of the new SCF approach for SCF-LOSC to correctly describe the electron densities, total energies, and energy-level alignment for the molecular dissociation process, while conventional DFAs or LOSC-DFAs with post-SCF calculations show large errors. This work demonstrates that the new SCF approach for SCF-LOSC would be a promising method for studying problems for correct electron densities and energy-level alignments in large systems.

Full Text

Duke Authors

Cited Authors

  • Mei, Y; Chen, Z; Yang, W

Published Date

  • December 2020

Published In

Volume / Issue

  • 11 / 23

Start / End Page

  • 10269 - 10277

PubMed ID

  • 33215928

Pubmed Central ID

  • 33215928

Electronic International Standard Serial Number (EISSN)

  • 1948-7185

International Standard Serial Number (ISSN)

  • 1948-7185

Digital Object Identifier (DOI)

  • 10.1021/acs.jpclett.0c03133

Language

  • eng