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6CCVD Research

Reduced Scaling of Optimal Regional Orbital Localization via Sequential Exhaustion of the Single-Particle Space

At a Glance

Section titled ā€œAt a Glanceā€
MetadataDetails
Publication Date2022-07-11
JournalJournal of Chemical Theory and Computation
AuthorsGuorong Weng, Mariya Romanova, Arsineh Apelian, Hanbin Song, Vojtěch Vlček
InstitutionsUniversity of California, Santa Barbara
Citations7

Abstract

Section titled ā€œAbstractā€

Wannier functions have become a powerful tool in the electronic structure calculations of extended systems. The generalized Pipek-Mezey Wannier functions exhibit appealing characteristics (e.g., reaching an optimal localization and the separation of the Ļƒ-Ļ€ orbitals) compared with other schemes. However, when applied to giant nanoscale systems, the orbital localization suffers from a large computational cost overhead if one is interested in localized states in a small fragment of the system. Herein, we present a swift, efficient, and robust approach for obtaining regionally localized orbitals of a subsystem within the generalized Pipek-Mezey scheme. The proposed algorithm introduces a reduced work space and sequentially exhausts the entire orbital space until the convergence of the localization functional. It tackles systems with āˆ¼10000 electrons within 0.5 h with no loss in localization quality compared to the traditional approach. Regionally localized orbitals with a higher extent of localization are obtained via judiciously extending the subsystemā€™s size. Exemplifying on large bulk and a 4 nm wide slab of diamond with an NV<sup>-</sup> center, we demonstrate the methodology and discuss how the choice of the localization region affects the excitation energy of the defect. Furthermore, we show how the sequential algorithm is easily extended to stochastic methodologies that do not provide individual single-particle eigenstates. It is thus a promising tool to obtain regionally localized states for solving the electronic structure problems of a subsystem embedded in giant condensed systems.

Tech Support

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Original Source

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References

Section titled ā€œReferencesā€
  1. 2011 - The LDA+DMFT approach to strongly correlated materials

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