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Environment-dependent tight-binding models from ab initio pseudoatomic orbital Hamiltonians

M. Buongiorno Nardelli

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Phys. Rev. B 114, 045125 – Published 24 July, 2026

DOI: https://doi.org/10.1103/y72v-hhxj

Abstract

Ab initio pseudoatomic orbital (PAO) Hamiltonians express the electronic structure of a solid in a compact, localized basis that spans the same Hilbert space as a conventional Slater-Koster tight-binding model, thereby providing an exact ab initio representation without any loss of accuracy. Building on this correspondence, we develop an environment-dependent tight-binding framework in which Slater-Koster hopping integrals are augmented with bond-screening functions that capture the local coordination environment. All parameters are determined by fitting to the PAO eigenvalue spectrum across multiple atomic configurations simultaneously, which breaks the degeneracy between screening and hopping parameters and yields physically meaningful, transferable models capable of generating Hamiltonians for large systems with ab initio precision. We demonstrate the efficiency and accuracy of the approach on four prototypical systems: bulk platinum, silicon surfaces, Si/Ge [001] superlattices, and twisted bilayer graphene with up to 4324 atoms. The method is implemented in the paoflow code and integrates seamlessly with its full postprocessing suite, enabling the evaluation of a broad range of electronic, optical, and transport properties.

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Phys. Rev. B 114, 045125– Published 24 July, 2026
  • Received 15 April 2026
  • Revised 12 June 2026
  • Accepted 8 July 2026
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Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.

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