Locality error free effective core potentials for 3d transition metal elements developed for the diffusion Monte...

Area of Science:

• Computational Materials Science
• Quantum Chemistry
• Condensed Matter Physics

Background:

• Diffusion Monte Carlo (DMC) is a powerful method for materials simulation.
• Pseudopotential locality errors limit DMC accuracy, especially for transition metal oxides.

Purpose of the Study:

• To develop locality error-free effective core potentials (pseudo-Hamiltonians) for transition metals (Cr-Zn).
• To improve the accuracy of many-body, first-principles calculations for complex materials.

Main Methods:

• Modified a previously established procedure for creating effective core potentials.
• Optimized pseudo-Hamiltonians to minimize transferability errors.
• Validated the new pseudo-Hamiltonians within the diffusion Monte Carlo framework.

Main Results:

• Developed a new set of locality error-free pseudo-Hamiltonians (OPH23) for transition metals.
• Achieved transferability errors comparable to state-of-the-art semilocal pseudopotentials.
• Demonstrated the potential to overcome limitations of previous methods.

Conclusions:

• The OPH23 set significantly enhances the accuracy of DMC calculations for transition metal-containing materials.
• This advancement is crucial for fundamental research in complex materials science.
• Enables more reliable first-principles simulations in condensed matter physics and chemistry.