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Title: Orbital spaces in the divide-expand-consolidate coupled cluster method

Abstract

The theoretical foundation for solving coupled cluster singles and doubles (CCSD) amplitude equations to a desired precision in terms of independent fragment calculations using restricted local orbital spaces is reinvestigated with focus on the individual error sources. Four different error sources are identified theoretically and numerically and it is demonstrated that, for practical purposes, local orbital spaces for CCSD calculations can be identified from calculations at the MP2 level. The development establishes a solid theoretical foundation for local CCSD calculations for the independent fragments, and thus for divide–expand–consolidate coupled cluster calculations for large molecular systems with rigorous error control. Based on this theoretical foundation, we have developed an algorithm for determining the orbital spaces needed for obtaining the single fragment energies to a requested precision and numerically demonstrated the robustness and precision of this algorithm

Authors:
 [1]; ORCiD logo [1];  [1];  [1];  [1]
  1. Aarhus Univ. (Denmark). qLEAP Center for Theoretical Chemistry, Dept. of Chemistry
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Oak Ridge Leadership Computing Facility (OLCF)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1565471
Alternate Identifier(s):
OSTI ID: 1421168
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 144; Journal Issue: 16; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
Chemistry; Physics

Citation Formats

Ettenhuber, Patrick, Baudin, Pablo, Kjærgaard, Thomas, Jørgensen, Poul, and Kristensen, Kasper. Orbital spaces in the divide-expand-consolidate coupled cluster method. United States: N. p., 2016. Web. doi:10.1063/1.4947019.
Ettenhuber, Patrick, Baudin, Pablo, Kjærgaard, Thomas, Jørgensen, Poul, & Kristensen, Kasper. Orbital spaces in the divide-expand-consolidate coupled cluster method. United States. doi:10.1063/1.4947019.
Ettenhuber, Patrick, Baudin, Pablo, Kjærgaard, Thomas, Jørgensen, Poul, and Kristensen, Kasper. Thu . "Orbital spaces in the divide-expand-consolidate coupled cluster method". United States. doi:10.1063/1.4947019. https://www.osti.gov/servlets/purl/1565471.
@article{osti_1565471,
title = {Orbital spaces in the divide-expand-consolidate coupled cluster method},
author = {Ettenhuber, Patrick and Baudin, Pablo and Kjærgaard, Thomas and Jørgensen, Poul and Kristensen, Kasper},
abstractNote = {The theoretical foundation for solving coupled cluster singles and doubles (CCSD) amplitude equations to a desired precision in terms of independent fragment calculations using restricted local orbital spaces is reinvestigated with focus on the individual error sources. Four different error sources are identified theoretically and numerically and it is demonstrated that, for practical purposes, local orbital spaces for CCSD calculations can be identified from calculations at the MP2 level. The development establishes a solid theoretical foundation for local CCSD calculations for the independent fragments, and thus for divide–expand–consolidate coupled cluster calculations for large molecular systems with rigorous error control. Based on this theoretical foundation, we have developed an algorithm for determining the orbital spaces needed for obtaining the single fragment energies to a requested precision and numerically demonstrated the robustness and precision of this algorithm},
doi = {10.1063/1.4947019},
journal = {Journal of Chemical Physics},
number = 16,
volume = 144,
place = {United States},
year = {2016},
month = {4}
}

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Cited by: 12 works
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