Designing 3d metal oxides: selecting optimal density functionals for strongly correlated materials.

Area of Science:

• Materials Science
• Computational Chemistry
• Solid-State Physics

Background:

• Transition metal oxides (TMOs) possess valuable physicochemical properties, making them ideal for technological applications.
• Density functional theory (DFT) is a powerful tool for understanding TMO properties and optimizing materials.
• Accurate description of localized 3d-electrons in TMOs necessitates careful selection of exchange-correlation (XC) functionals.

Purpose of the Study:

• To benchmark various density functionals (DFs) for describing 3d TMO properties.
• To compare DFT predictions with experimental magneto-electro-optical data.
• To identify the most reliable XC functional for TMO electronic structure calculations.

Main Methods:

• Systematic evaluation of DFs from GGA to RSH using the def2-TZVP basis set.
• Analysis of electronic, optical, magnetic, and structural properties.
• Assessment of computational cost and spin contamination.

Main Results:

• The study reveals the varying accuracy and efficiency of different XC functionals.
• PBE0-1/5 emerged as the top-performing functional for 3d TMOs.
• Key properties like band structure, density of states, and magnetic moments were analyzed.

Conclusions:

• The choice of XC functional significantly impacts the accuracy of DFT in TMOs.
• PBE0-1/5 offers a trustworthy description of the ground-state electron structure for 3d TMOs.
• This work guides the selection of XC functionals for future materials science modeling.