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.
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28 March 2023
Research Article|
March 30 2023
Scaled opposite-spin atomic-orbital based algebraic diagrammatic construction scheme for the polarization propagator with asymptotic linear-scaling effort: Theory and implementation
M. A. Ambroise
;
M. A. Ambroise
(Conceptualization, Data curation, Formal analysis, Investigation, Software, Validation, Writing – original draft)
1
Interdisciplinary Center for Scientific Computing, Ruprecht-Karls University
, Im Neuenheimer Feld 205, 69120 Heidelberg, Germany
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F. Sacchetta
;
F. Sacchetta
(Conceptualization, Data curation, Formal analysis, Methodology, Software, Validation, Writing – original draft)
2
Chair of Theoretical Chemistry, Department of Chemistry, University of Munich (LMU)
, D-81377 Munich, Germany
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D. Graf
;
D. Graf
(Conceptualization, Data curation, Formal analysis, Supervision, Writing – original draft, Writing – review & editing)
2
Chair of Theoretical Chemistry, Department of Chemistry, University of Munich (LMU)
, D-81377 Munich, Germany
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C. Ochsenfeld
;
C. Ochsenfeld
(Conceptualization, Formal analysis, Funding acquisition, Methodology, Resources, Supervision, Writing – review & editing)
2
Chair of Theoretical Chemistry, Department of Chemistry, University of Munich (LMU)
, D-81377 Munich, Germany
3
Max Planck Institute for Solid State Research
, 70569 Stuttgart, Germany
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A. Dreuw
A. Dreuw
a)
(Conceptualization, Funding acquisition, Project administration, Resources, Supervision, Writing – review & editing)
1
Interdisciplinary Center for Scientific Computing, Ruprecht-Karls University
, Im Neuenheimer Feld 205, 69120 Heidelberg, Germany
a)Author to whom correspondence should be addressed: [email protected]
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a)Author to whom correspondence should be addressed: [email protected]
J. Chem. Phys. 158, 124121 (2023)
Article history
Received:
December 24 2022
Accepted:
March 09 2023
Citation
M. A. Ambroise, F. Sacchetta, D. Graf, C. Ochsenfeld, A. Dreuw; Scaled opposite-spin atomic-orbital based algebraic diagrammatic construction scheme for the polarization propagator with asymptotic linear-scaling effort: Theory and implementation. J. Chem. Phys. 28 March 2023; 158 (12): 124121. https://doi.org/10.1063/5.0139894
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