Wannier Function Localization Using Bloch Intrinsic Atomic Orbitals

• Published in: The journal of physical chemistry. A, Molecules, spectroscopy, kinetics, environment, & general theory Vol. 128; no. 39; pp. 8570 - 8579
• Main Authors: Zhu, Andrew, Tew, David P.
• Format: Journal Article
• Language: English
• Published: United States American Chemical Society 03.10.2024
• Subjects: A: New Tools and Methods in Experiment and Theory
• ISSN: 1089-5639; 1520-5215; 1520-5215
• DOI: 10.1021/acs.jpca.4c04555

We extend the intrinsic atomic orbital (IAO) method for the localization of molecular orbitals to calculate well-localized generalized Wannier functions in crystals in the spirit of the Pipek–Mezey method. We furthermore present a one-shot diabatic Wannierization procedure that aligns the phases of the Bloch functions, providing immediate Wannier localization, which serves as an excellent initial guess for optimization. We test our Wannier localization implementation on a number of solid-state systems, highlighting the effectiveness of the diabatic preparation, especially for localizing core bands. Partial charges of Wannier functions generated using Bloch IAOs align well with chemical intuition, which we demonstrate through the example of the adsorption of CO on a MgO surface.