Screened-exchange density functionals with broad accuracy for chemistry and solid-state physics.

Area of Science:

• Computational Chemistry
• Quantum Chemistry
• Materials Science

Background:

• Hybrid Kohn-Sham methods are crucial for accurate electronic structure calculations.
• Existing functionals like N12 and MN12-L have limitations in describing electron exchange interactions.
• Screened Hartree-Fock exchange offers a promising avenue for improving functional accuracy.

Purpose of the Study:

• To introduce and evaluate two novel exchange-correlation functionals: N12-SX and MN12-SX.
• To assess the impact of incorporating screened Hartree-Fock exchange into hybrid functionals.
• To compare the performance of the new functionals against established methods.

Main Methods:

• Development of N12-SX (density and density gradient dependent) and MN12-SX (density, density gradient, and kinetic energy density dependent) functionals.
• Inclusion of short-range Hartree-Fock exchange, screened at long-range.
• Comparative accuracy assessment against N12, MN12-L, HSE06, global-hybrid GGA, and long-range-corrected meta-GGA functionals.

Main Results:

• N12-SX and MN12-SX functionals demonstrate improved accuracy in electronic structure calculations.
• The addition of screened exchange significantly impacts functional performance.
• Performance of the new functionals is competitive with or superior to existing state-of-the-art methods.

Conclusions:

• N12-SX and MN12-SX represent significant advancements in exchange-correlation functional development.
• These functionals offer a more accurate and reliable approach for hybrid Kohn-Sham calculations.
• The screened exchange approach is validated as an effective strategy for improving computational chemistry predictions.