Development of a joint refinement model for the spin-resolved one-electron reduced density matrix using different...

Area of Science:

• Quantum Chemistry
• Materials Science
• Solid State Physics

Background:

• Accurate determination of the spin-resolved one-electron reduced density matrix is crucial for understanding magnetic properties.
• Existing methods often rely on limited experimental data, potentially leading to inaccuracies.

Purpose of the Study:

• To develop and validate a joint refinement model for the spin-resolved one-electron reduced density matrix.
• To assess the impact of simultaneously using magnetic structure factors and magnetic directional Compton profiles.

Main Methods:

• A joint refinement model was developed, incorporating variations in basis functions and the spin population matrix.
• The model's implementation for finite systems utilizes an expansion of natural orbitals on basis sets.
• Comparison with a model using only magnetic structure factors was performed.

Main Results:

• The joint refinement model yielded highly satisfactory results, accurately reproducing pseudo-data.
• Magnetic Compton profiles were found to significantly influence both diagonal and off-diagonal elements of the spin-resolved one-electron reduced density matrix.
• The joint model demonstrated superior performance compared to using magnetic structure factors alone.

Conclusions:

• The joint refinement model offers a more robust and accurate method for determining the spin-resolved one-electron reduced density matrix.
• Simultaneous use of magnetic structure factors and magnetic Compton profiles is essential for a comprehensive description of magnetic electronic structure.