Long-range corrected density functional theory with accelerated Hartree-Fock exchange integration using a...

Area of Science:

• Quantum Chemistry
• Computational Materials Science

Background:

• Hybrid functionals are essential for molecular system calculations.
• Long-range corrected hybrid schemes enhance accuracy but are computationally expensive.
• Hartree-Fock (HF) exchange integral evaluation is a major bottleneck.

Purpose of the Study:

• To develop a computationally efficient method for long-range corrected hybrid schemes.
• To address the high computational cost of HF exchange integrals in large systems.

Main Methods:

• Proposed a modified two-Gaussian attenuating operator.
• Replaced the error function for long-range HF exchange integral computation.
• Utilized periodic boundary conditions for large system calculations (e.g., C diamond).

Main Results:

• Achieved dramatic reduction in computational time (e.g., ~14x acceleration).
• Demonstrated lower computational scaling with increasing system size.
• Maintained the accuracy and improved features of long-range corrected density functional theory.

Conclusions:

• The proposed two-Gaussian HF operator offers a significant speed-up for hybrid functional calculations.
• This method makes hybrid functionals more applicable to large molecular and periodic systems.
• Enables broader and more active applications of advanced quantum chemical methods.