The quantum Monte Carlo (QMC) algebraic diagrammatic construction (ADC) method is introduced, which solves the eigenvalue problem of the second-order ADC scheme for the polarization propagator stochastically within the framework of QMC methodology allowing for massively parallel computations. As common virtue of the Monte Carlo integration techniques, quantum Monte Carlo algebraic diagrammatic construction (QMCADC) enables exploitation of the sparsity of the effective ADC matrix, and it reduces the memory requirements by storing only a portion of configurations at each iteration. Furthermore, distributing memory and processing loads to different computing nodes enables the use of fast developing parallel computing resources. Here, the theory and implementation of QMCADC is reported and its viability is demonstrated by the first proof-of-principle calculations. The focus lies on the first excited state and the reproduction of the corresponding lowest vertical excitation energy of various molecular systems. QMCADC is shown to be a genuine stochastic solution of the ADC eigenvalue problem, and exact ADC values can be obtained with a marginal controllable error.
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28 January 2022
Research Article|
January 24 2022
Quantum Monte Carlo formulation of the second order algebraic diagrammatic construction: Toward a massively parallel correlated excited state method
Adem Halil Kulahlioglu
;
Adem Halil Kulahlioglu
Interdisciplinary Center for Scientific Computing, Ruprecht-Karls University
, Im Neuenheimer Feld 205, 69120 Heidelberg, Germany
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Dirk Rehn
;
Dirk Rehn
Interdisciplinary Center for Scientific Computing, Ruprecht-Karls University
, Im Neuenheimer Feld 205, 69120 Heidelberg, Germany
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Andreas Dreuw
Andreas Dreuw
a)
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. 156, 044105 (2022)
Article history
Received:
September 11 2021
Accepted:
December 31 2021
Citation
Adem Halil Kulahlioglu, Dirk Rehn, Andreas Dreuw; Quantum Monte Carlo formulation of the second order algebraic diagrammatic construction: Toward a massively parallel correlated excited state method. J. Chem. Phys. 28 January 2022; 156 (4): 044105. https://doi.org/10.1063/5.0071091
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