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

Abstract

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.

Authors:
ORCiD logo [1];  [2]; ORCiD logo [3]; ORCiD logo [4]; ORCiD logo [5]
  1. Univ. of Minnesota, Minneapolis, MN (United States); Univ. of Tennessee, Knoxville, TN (United States)
  2. Univ. of Minnesota, Minneapolis, MN (United States); Max Planck Institut fur Festkorperforschung, Stuttgart (Germany)
  3. Aarhus Univ., Aarhus C (Denmark)
  4. Univ. of Minnesota, Minneapolis, MN (United States)
  5. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
SC-22.1 USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division; USDOE
OSTI Identifier:
1436649
Alternate Identifier(s):
OSTI ID: 1420593
Grant/Contract Number:  
AC02-05CH11231; SC0008666
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 147; Journal Issue: 18; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Vogiatzis, Konstantinos D., Ma, Dongxia, Olsen, Jeppe, Gagliardi, Laura, and de Jong, Wibe A. Pushing configuration-interaction to the limit: Towards massively parallel MCSCF calculations. United States: N. p., 2017. Web. doi:10.1063/1.4989858.
Vogiatzis, Konstantinos D., Ma, Dongxia, Olsen, Jeppe, Gagliardi, Laura, & de Jong, Wibe A. Pushing configuration-interaction to the limit: Towards massively parallel MCSCF calculations. United States. doi:10.1063/1.4989858.
Vogiatzis, Konstantinos D., Ma, Dongxia, Olsen, Jeppe, Gagliardi, Laura, and de Jong, Wibe A. Tue . "Pushing configuration-interaction to the limit: Towards massively parallel MCSCF calculations". United States. doi:10.1063/1.4989858. https://www.osti.gov/servlets/purl/1436649.
@article{osti_1436649,
title = {Pushing configuration-interaction to the limit: Towards massively parallel MCSCF calculations},
author = {Vogiatzis, Konstantinos D. and Ma, Dongxia and Olsen, Jeppe and Gagliardi, Laura and de Jong, Wibe A.},
abstractNote = {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.},
doi = {10.1063/1.4989858},
journal = {Journal of Chemical Physics},
number = 18,
volume = 147,
place = {United States},
year = {2017},
month = {11}
}

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