Eliminating delocalization error through localized orbital scaling correction with orbital relaxation from linear...

Area of Science:

• Computational Chemistry
• Quantum Chemistry
• Materials Science

Background:

• Kohn-Sham density functional theory (KS-DFT) is widely used but suffers from delocalization errors.
• These errors lead to inaccuracies in calculated ionization energies, electron affinities, band structures, and charge distributions.
• Localized orbital scaling correction (LOSC) methods aim to mitigate these errors.

Purpose of the Study:

• To extend the applicability of the linear response localized orbital scaling correction (lrLOSC) method to a wider range of molecular systems.
• To focus on corrections to valence orbital energies and total energies in various molecular sizes.
• To develop an efficient implementation of lrLOSC for large chemical systems.

Main Methods:

• The study utilizes the linear response localized orbital scaling correction (lrLOSC) method.
• An efficient implementation of lrLOSC was developed for computational efficiency.
• The method incorporates a functional correction including screening effects and orbital localization.

Main Results:

• The efficient lrLOSC implementation achieves computational costs comparable to standard KS-DFT.
• Screening effects are crucial for high accuracy in larger molecules, offering modest improvements for small ones.
• lrLOSC accurately describes valence orbital energies and total energies across various molecular sizes.

Conclusions:

• The lrLOSC method, with its efficient implementation, accurately describes a broad spectrum of chemical systems.
• It provides reliable computational simulations for organic molecules and transition-metal oxide complexes.
• lrLOSC is established as a powerful tool for enhancing the accuracy of computational chemistry.