Self-consistent density-based basis-set correction: How much do we lower total energies and improve dipole moments?

Area of Science:

• Computational chemistry
• Quantum chemistry
• Electronic structure theory

Background:

• Density-based basis-set correction methods improve wave function calculations.
• Previous approximations added corrections post-calculation.

Purpose of the Study:

• To develop and test a self-consistent extension of the density-based basis-set correction method.
• To evaluate the impact on total energy and molecular properties like dipole moments.

Main Methods:

• Implemented a self-consistent energy minimization including basis-set corrections.
• Tested two basis-set correction functionals on various molecular systems.

Main Results:

• Self-consistent approach yields negligible total energy lowering compared to non-self-consistent methods.
• Basis-set corrected wave functions significantly improve dipole moment accuracy, nearing complete basis-set limit.

Conclusions:

• The non-self-consistent approximation is justified due to minimal energy differences.
• The self-consistent density-based basis-set correction scheme is robust and enhances property prediction.