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arXiv · 2610.00123

Strictly Localized Molecular Orbitals: Non-Orthogonal Local Orbitals Built with Chemical Intuition

Jeffrey Keyes·Carlos Jimenez-Hoyos
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Abstract

We propose the use of an a priori localization method based on separating the molecule into fragments to generate a wavefunction suitable for post Hartree-Fock methods. A quasi-Newton approach utilizing Thouless rotation is developed to optimize the strictly localized molecular orbitals(sLMO). We discuss the properties of the sLMO-HF wavefunction and compare it to the tail deleted a posteriori localization methods that are usually done in preparation of post Hartree-Fock methods. We then discuss the effects of choosing different fragmentation patterns and basis sets.

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Jeffrey Keyes, Carlos Jimenez-Hoyos. 2026-09-09. Strictly Localized Molecular Orbitals: Non-Orthogonal Local Orbitals Built with Chemical Intuition. https://arxiv.org/abs/2610.00123

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