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arXiv · 2610.23005

Low-Cost Third-order Algebraic Diagrammatic Construction Method for Excited States Using Tensor Hypercontraction and State-Specific Frozen Natural Orbitals

Amrita Manna·Sudipta Chakraborty·Alexander B. Trofimov·Alexander Yu. Sokolov·Achintya Kumar Dutta
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Abstract

We have developed a reduced-cost framework for excited-state calculations by combining the state-specific frozen natural orbital (SS-FNO) approach with the third-order algebraic diagrammatic construction [ADC(3)] method and tensor hypercontraction (THC). This strategy enables a systematic and controllable truncation of the virtual orbital space, while significantly lowering the computational scaling through the THC representation of the electron repulsion integrals. The method allows black-box application via adjustable thresholds and includes a perturbative correction that compensates for the truncation error. We have used the CIS(D) method to generate the natural orbitals for the excited states. The performance of the SS-FNO-THC-ADC(3) method is assessed for valence, Rydberg, and charge-transfer excitations. Benchmark calculations demonstrate that the combined approach achieves excellent agreement with the canonical ADC(3) results. The efficiency of the present implementation is demonstrated by calculating the excitation energy of a molecule containing 31 atoms and more than one thousand basis functions.

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Amrita Manna, Sudipta Chakraborty, Alexander B. Trofimov, Alexander Yu. Sokolov, Achintya Kumar Dutta. 2026-10-16. Low-Cost Third-order Algebraic Diagrammatic Construction Method for Excited States Using Tensor Hypercontraction and State-Specific Frozen Natural Orbitals. https://arxiv.org/abs/2610.23005

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