A Third-Order Relativistic Algebraic Diagrammatic Construction Method for Double Ionization Potentials: Theory, Implementation, and Benchmark

Fuente: arXiv
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Main Authors: Mandal, Sujan, Dutta, Achintya Kumar
Format: Preprint
Published: 2025
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author Mandal, Sujan
Dutta, Achintya Kumar
author_facet Mandal, Sujan
Dutta, Achintya Kumar
contents We present a relativistic third-order algebraic diagrammatic construction (ADC(3)) approach for calculating double ionization potentials (DIPs). By employing the exact two-component atomic mean-field (X2CAMF) Hamiltonian in combination with a Cholesky decomposition (CD) representation of two-electron integrals and the frozen natural spinor (FNS) framework for virtual space truncation, we achieve a significant reduction in both memory requirements and computational cost. The DIPs obtained using the X2CAMF Hamiltonian show excellent agreement with results from fully relativistic four-component calculations. We have validated the accuracy of our implementation through comparisons with available experimental and theoretical data for inert gas atoms and diatomic species. The effect of higher-order relativistic corrections is also explored.
format Preprint
id arxiv_https___arxiv_org_abs_2508_19012
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle A Third-Order Relativistic Algebraic Diagrammatic Construction Method for Double Ionization Potentials: Theory, Implementation, and Benchmark
Mandal, Sujan
Dutta, Achintya Kumar
Chemical Physics
We present a relativistic third-order algebraic diagrammatic construction (ADC(3)) approach for calculating double ionization potentials (DIPs). By employing the exact two-component atomic mean-field (X2CAMF) Hamiltonian in combination with a Cholesky decomposition (CD) representation of two-electron integrals and the frozen natural spinor (FNS) framework for virtual space truncation, we achieve a significant reduction in both memory requirements and computational cost. The DIPs obtained using the X2CAMF Hamiltonian show excellent agreement with results from fully relativistic four-component calculations. We have validated the accuracy of our implementation through comparisons with available experimental and theoretical data for inert gas atoms and diatomic species. The effect of higher-order relativistic corrections is also explored.
title A Third-Order Relativistic Algebraic Diagrammatic Construction Method for Double Ionization Potentials: Theory, Implementation, and Benchmark
topic Chemical Physics
url https://arxiv.org/abs/2508.19012