Pushing configuration-interaction to the limit: Towards massively parallel MCSCF calculations

Vogiatzis, Konstantinos D.; Ma, Dongxia; Olsen, Jeppe; Gagliardi, Laura; de Jong, Wibe A.

doi:10.1063/1.4989858

Title: Pushing configuration-interaction to the limit: Towards massively parallel MCSCF calculations

Journal Article · Tue Nov 14 00:00:00 EST 2017 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.4989858· OSTI ID:1436649

^[1]; Ma, Dongxia ^[2];

^[3];

^[4];

^[5]

Univ. of Minnesota, Minneapolis, MN (United States); Univ. of Tennessee, Knoxville, TN (United States)
Univ. of Minnesota, Minneapolis, MN (United States); Max Planck Institut fur Festkorperforschung, Stuttgart (Germany)
Aarhus Univ., Aarhus C (Denmark)
Univ. of Minnesota, Minneapolis, MN (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

A new large-scale parallel multiconfigurational self-consistent field (MCSCF) implementation in the open-source NWChem computational chemistry code is presented. The generalized active space approach is used to partition large configuration interaction (CI) vectors and generate a sufficient number of batches that can be distributed to the available cores. Massively parallel CI calculations with large active spaces can be performed. The new parallel MCSCF implementation is tested for the chromium trimer and for an active space of 20 electrons in 20 orbitals, which can now routinely be performed. Unprecedented CI calculations with an active space of 22 electrons in 22 orbitals for the pentacene systems were performed and a single CI iteration calculation with an active space of 24 electrons in 24 orbitals for the chromium tetramer was possible. In conclusion, the chromium tetramer corresponds to a CI expansion of one trillion Slater determinants (914 058 513 424) and is the largest conventional CI calculation attempted up to date.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: SC-22.1 USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division; USDOE

Grant/Contract Number:: AC02-05CH11231; SC0008666

OSTI ID:: 1436649

Alternate ID(s):: OSTI ID: 1420593

Journal Information:: Journal of Chemical Physics, Vol. 147, Issue 18; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 103 works

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