Optimized Non-Orthogonal Localized Orbitals for Electronic Structure Calculations: Improved Linear Scaling Quantum Monte Carlo

2004/07/07 by Fernando A. Reboredo, F. A. Reboredo, Reboredo, F. A. +3
Chemical Engineering · Materials Science · Physics and Astronomy · #Advanced Chemical Physics Studies #Catalysis and Oxidation Reactions #FOS: Physical sciences #Machine Learning in Materials Science #Materials Science (cond-mat.mtrl-sci) #cond-mat.mtrl-sci

paper · pdf · doi:10.48550/arxiv.cond-mat/0407184

arxiv created 2004/07/07 · openalex publication_date 2004/07/07 · arxiv updated 2009/12/01 · openalex created_date 2025/10/10 · openalex updated_date 2026/08/01

Abstract

We derive an automatic procedure for generating a set of highly localized, non-orthogonal orbitals for linear scaling quantum Monte Carlo calculations. We demonstrate the advantage of these orbitals in calculations of the total energy of both semiconducting and metallic systems by studying bulk silicon and the homogeneous electron gas. For silicon, the improved localization of these orbitals reduces the computational time by a factor five and the memory by a factor of six compared to localized, orthogonal orbitals. For jellium, we demonstrate that the total energy is converged for orbitals truncated within spheres with radii 7-8 r_s, opening the possibility of linear scaling QMC calculations for realistic metallic systems.

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