Efficient and Parallel Implementation of Real and Complex Response Functions Employing the Second-Order Algebraic-Diagrammatic Construction Scheme for the Polarization Propagator

QC 20240122
We present the implementation of an efficient matrix-folded formalism for the evaluation of complex response functions and the calculation of transition properties at the level of the second-order algebraic-diagrammatic construction (ADC(2)) scheme. The underlying algorithms, in combination with the adopted hybrid MPI/OpenMP parallelization strategy, enabled calculations of the UV/vis spectra of a guanine oligomer series ranging up to 1032 contracted basis functions, thereby utilizing vast computational resources from up to 32,768 CPU cores. Further analysis of the convergence behavior of the involved iterative subspace algorithms revealed the superiority of a frequency-separated treatment of response equations even for a large spectral window, including 101 frequencies. We demonstrate the applicability to general quantum mechanical operators by the first reported electronic circular dichroism spectrum calculated with a complex polarization propagator approach at the ADC(2) level of theory.

Dreuw, AndreasRuprecht Karls Univ Heidelberg, Interdisciplinary Ctr Sci Comp, D-69120 Heidelberg, Germany. (author)
Norman, PatrickKTH,Teoretisk kemi och biologi(Swepub:kth)u1c4e2k0 (author)
Li, XinKTH,Parallelldatorcentrum, PDC(Swepub:kth)u1omz1ee (author)
KTHTeoretisk kemi och biologi (creator_code:org_t)

In:Journal of Chemical Theory and Computation: American Chemical Society (ACS)20:1, s. 103-1131549-96181549-9626

By the author/editor: Brand, Manuel; Dreuw, Andreas; Norman, Patrick; Li, Xin

About the subject

NATURAL SCIENCES: NATURAL SCIENCES; and Chemical Science ...; and Theoretical Chem ...

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