Simple and Efficient Route toward Improved Energetics within the Framework of Density-Corrected Density Functional...

Area of Science:

• Quantum Chemistry
• Computational Materials Science
• Theoretical Physics

Background:

• Density-corrected Hartree-Fock density functional theory (DC(HF)-DFT) requires identifying erroneous densities from density functionals.
• Accurate electron density is crucial for reliable electronic structure calculations.

Purpose of the Study:

• Introduce a novel indicator to reliably detect when Hartree-Fock (HF) density is superior to density functional theory (DFT) density.
• Develop an efficient procedure to correct both the electron density and the functional in DC(HF)-DFT calculations.

Main Methods:

• A new indicator based on the difference in non-interacting kinetic energies between DFT and HF calculations is proposed.
• The indicator directly compares self-consistent DFT density with HF density.
• A procedure evaluating a related hybrid functional is introduced to correct the functional alongside the density.

Main Results:

• The kinetic energy indicator is size-intensive, reliable, and highly efficient.
• The proposed indicator accurately determines the necessity of using HF density.
• The C(HF)-DFT procedure corrects both density and functional.

Conclusions:

• The developed kinetic energy indicator provides an efficient and reliable way to improve DC(HF)-DFT.
• The C(HF)-DFT procedure offers a more comprehensive correction by refining both density and functional, enhancing accuracy in electronic structure predictions.