Hybrid Atomic Orbital Basis from First Principles: Bottom-Up Mapping of Self-Energy Correction to Large Covalent...

Area of Science:

• Computational Materials Science
• Quantum Chemistry
• Solid-State Physics

Background:

• Accurate electronic structure calculations are crucial for understanding material properties.
• Traditional methods can be computationally expensive for large systems.
• Developing efficient and transferable basis sets is an ongoing challenge.

Purpose of the Study:

• To introduce a novel construction of hybrid atomic orbitals as a basis set.
• To enable efficient and accurate calculation of electronic structures for large covalent systems.
• To facilitate the transferability of parameters across similar material structures.

Main Methods:

• Construction of hybrid atomic orbitals as approximate common eigenstates of finite first moment matrices.
• Development of Wannier function counterparts from Kohn-Sham (KS) single-particle states.
• Creation of an orthonormal multiorbital tight-binding (TB) basis set.

Main Results:

• The proposed TB basis set allows for predominantly single TB parameters per nearest neighbor bond.
• The spatial extent of self-energy correction (SEC) is localized within the third nearest neighborhood.
• Effective transfer of self-energy-corrected TB parameters between systems of varying sizes is demonstrated.

Conclusions:

• The proposed method offers an inexpensive yet accurate approach for estimating quasi-particle structures.
• This method significantly reduces computational cost for large covalent systems.
• The developed TB basis set shows promise for efficient materials modeling.