Spin-Polarized Conceptual Density Functional Theory from the Convex Hull

Area of Science:

• Quantum Chemistry
• Theoretical Chemistry
• Materials Science

Background:

• Conceptual Density-Functional Theory (DFT) provides fundamental insights into chemical reactivity.
• Spin-polarized systems require specialized theoretical frameworks for accurate description.
• Existing SP-DFT models lack a consistent and unambiguous foundation.

Purpose of the Study:

• To establish a rigorous and internally consistent framework for spin-polarized conceptual DFT (SP-DFT).
• To develop continuous energy models for SP-DFT calculations.
• To generalize key conceptual DFT reactivity indices, such as Parr functions, to spin-polarized systems.

Main Methods:

• Characterization of the energy convex hull as the defining feature of ground states in SP-DFT.
• Construction of continuous linear and quadratic energy models based on the energy hull.
• Generalization of Parr functions and their derivatives within the new SP-DFT framework.

Main Results:

• A nonarbitrary, internally consistent framework for SP-DFT is presented.
• Continuous linear and quadratic energy models accurately represent the energy landscape.
• The generalized Parr functions offer new insights into spin-polarized reactivity.

Conclusions:

• The developed SP-DFT framework offers a robust foundation for studying spin-polarized chemical systems.
• The continuous energy models and generalized Parr functions enhance the predictive power of conceptual DFT.
• This work integrates spin-polarization seamlessly into the conceptual DFT paradigm.