Workhorse semilocal density functional for condensed matter physics and quantum chemistry

Area of Science:

• Computational chemistry
• Materials science
• Quantum mechanics

Background:

• Semilocal density functionals are crucial for large electronic systems.
• The Tao-Perdew-Staroverov-Scuseria (TPSS) meta-generalized gradient approximation (meta-GGA) is accurate but overestimates lattice constants.
• Existing "GGA’s for solids" provide accurate lattice constants but fail for molecular atomization energies.

Purpose of the Study:

• To develop a revised meta-generalized gradient approximation (meta-GGA) functional.
• To address the limitations of existing functionals in predicting both lattice constants and atomization energies.
• To achieve accurate predictions for ordinary matter properties.

Main Methods:

• Utilizing the construction principle of "GGA’s for solids" by restoring the density gradient expansion for exchange.
• Modifying the Tao-Perdew-Staroverov-Scuseria (TPSS) meta-GGA.
• Testing the revised functional against established benchmarks for lattice constants, surface energies, and atomization energies.

Main Results:

• The revised TPSS meta-GGA yields accurate lattice constants, comparable to "GGA’s for solids".
• The new functional demonstrates improved accuracy for molecular atomization energies.
• The revised TPSS meta-GGA successfully predicts surface energies for ordinary matter.

Conclusions:

• A revised TPSS meta-GGA functional offers a balanced and accurate approach for electronic system calculations.
• This development overcomes the trade-off between accurate lattice constants and atomization energies in previous functionals.
• The revised functional is suitable for predicting diverse properties of ordinary matter.