Scaled opposite-spin atomic-orbital based algebraic diagrammatic construction scheme for the polarization propagator with asymptotic linear-scaling effort

• Verfasst von: Ambroise, Maximilien [VerfasserIn]
• Verfasst von: Sacchetta, Filippo [VerfasserIn]
• Verfasst von: Graf, Daniel [VerfasserIn]
• Verfasst von: Ochsenfeld, C. [VerfasserIn]
• Verfasst von: Dreuw, Andreas [VerfasserIn]
• Titel: Scaled opposite-spin atomic-orbital based algebraic diagrammatic construction scheme for the polarization propagator with asymptotic linear-scaling effort
• Titelzusatz: theory and implementation
• Verf.angabe: M.A. Ambroise, F. Sacchetta, D. Graf, C. Ochsenfeld, and A. Dreuw
• E-Jahr: 2023
• Jahr: 30 March 2023
• Umfang: 16 S.
• Fussnoten: Gesehen am 17.05.2023
• Titel Quelle: Enthalten in: The journal of chemical physics
• Ort Quelle: Melville, NY : American Institute of Physics, 1933
• Jahr Quelle: 2023
• Band/Heft Quelle: 158(2023), 12 vom: März, Artikel-ID 124121, Seite 1-16
• ISSN Quelle: 1089-7690
• DOI: doi:10.1063/5.0139894
• Datenträger: Online-Ressource
• Sprache: eng
• K10plus-PPN: 1845603885

Abstract

A novel local approach for the quantum-chemical computation of excited states is presented, where the concept of the atomic-orbital formulation of the second-order Møller-Plesset energy expression is extended to the second-order algebraic diagrammatic construction scheme by virtue of the Laplace transform. The scaled opposite-spin second-order algebraic diagrammatic construction method with Cholesky decomposed densities and density-fitting, or CDD-DF-SOS-ADC(2) for short, exploits the sparsity of the two-electron repulsion integrals, the atomic ground-state density matrix, and the atomic transition density matrix to drastically reduce the computational effort. By using a local density-fitting approximation, it is shown that asymptotically linear scaling can be achieved for linear carboxylic acids. For electron-dense systems, sub-cubic scaling can be achieved if the excitation is local, and hence the transition density is sparse. Furthermore, the memory footprint and accuracy of the CDD-DF-SOS-ADC(2) method are explored in detail.