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Title: Improved treatment of exact exchange in Quantum ESPRESSO

Abstract

© 2017 We present an algorithm and implementation for the parallel computation of exact exchange in Quantum ESPRESSO (QE) that exhibits greatly improved strong scaling. QE is an open-source software package for electronic structure calculations using plane wave density functional theory, and supports the use of local, semi-local, and hybrid DFT functionals. Wider application of hybrid functionals is desirable for the improved simulation of electronic band energy alignments and thermodynamic properties, but the computational complexity of evaluating the exact exchange potential limits the practical application of hybrid functionals to large systems and requires efficient implementations. We demonstrate that existing implementations of hybrid DFT that utilize a single data structure for both the local and exact exchange regions of the code are significantly limited in the degree of parallelization achievable. We present a band-pair parallelization approach, in which the calculation of exact exchange is parallelized and evaluated independently from the parallelization of the remainder of the calculation, with the wavefunction data being efficiently transformed on-the-fly into a form that is optimal for each part of the calculation. For a 64 water molecule supercell, our new algorithm reduces the overall time to solution by nearly an order of magnitude.

Authors:
 [1];  [1];  [2];  [2];  [1]; ORCiD logo [3];  [1]
+ Show Author Affiliations
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  2. Cray Inc., Saint Paul, MN (United States)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Advanced Scientific Computing Research (ASCR)
OSTI Identifier:
1376349
Alternate Identifier(s):
OSTI ID: 1379829; OSTI ID: 1396579
Grant/Contract Number:  
AC05-00OR22725; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Computer Physics Communications
Additional Journal Information:
Journal Volume: 214; Journal Issue: C; Journal ID: ISSN 0010-4655
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
97 MATHEMATICS AND COMPUTING; Hybrid DFT; Quantum ESPRESSO; Scalability

Citation Formats

Barnes, Taylor A., Kurth, Thorsten, Carrier, Pierre, Wichmann, Nathan, Prendergast, David, Kent, Paul R. C., and Deslippe, Jack. Improved treatment of exact exchange in Quantum ESPRESSO. United States: N. p., 2017. Web. doi:10.1016/j.cpc.2017.01.008.
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Barnes, Taylor A., Kurth, Thorsten, Carrier, Pierre, Wichmann, Nathan, Prendergast, David, Kent, Paul R. C., & Deslippe, Jack. Improved treatment of exact exchange in Quantum ESPRESSO. United States. https://doi.org/10.1016/j.cpc.2017.01.008
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Barnes, Taylor A., Kurth, Thorsten, Carrier, Pierre, Wichmann, Nathan, Prendergast, David, Kent, Paul R. C., and Deslippe, Jack. Wed . "Improved treatment of exact exchange in Quantum ESPRESSO". United States. https://doi.org/10.1016/j.cpc.2017.01.008. https://www.osti.gov/servlets/purl/1376349.
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@article{osti_1376349,
title = {Improved treatment of exact exchange in Quantum ESPRESSO},
author = {Barnes, Taylor A. and Kurth, Thorsten and Carrier, Pierre and Wichmann, Nathan and Prendergast, David and Kent, Paul R. C. and Deslippe, Jack},
abstractNote = {© 2017 We present an algorithm and implementation for the parallel computation of exact exchange in Quantum ESPRESSO (QE) that exhibits greatly improved strong scaling. QE is an open-source software package for electronic structure calculations using plane wave density functional theory, and supports the use of local, semi-local, and hybrid DFT functionals. Wider application of hybrid functionals is desirable for the improved simulation of electronic band energy alignments and thermodynamic properties, but the computational complexity of evaluating the exact exchange potential limits the practical application of hybrid functionals to large systems and requires efficient implementations. We demonstrate that existing implementations of hybrid DFT that utilize a single data structure for both the local and exact exchange regions of the code are significantly limited in the degree of parallelization achievable. We present a band-pair parallelization approach, in which the calculation of exact exchange is parallelized and evaluated independently from the parallelization of the remainder of the calculation, with the wavefunction data being efficiently transformed on-the-fly into a form that is optimal for each part of the calculation. For a 64 water molecule supercell, our new algorithm reduces the overall time to solution by nearly an order of magnitude.},
doi = {10.1016/j.cpc.2017.01.008},
journal = {Computer Physics Communications},
number = C,
volume = 214,
place = {United States},
year = {Wed Jan 18 00:00:00 EST 2017},
month = {Wed Jan 18 00:00:00 EST 2017}
}
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https://doi.org/10.1016/j.cpc.2017.01.008
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    Works referencing / citing this record:

    Pervasive Delocalisation Error Causes Spurious Proton Transfer in Organic Acid-Base Co-Crystals
    journal, October 2018

    • LeBlanc, Luc M.; Dale, Stephen G.; Taylor, Christopher R.
    • Angewandte Chemie, Vol. 130, Issue 45
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    Fast hybrid density-functional computations using plane-wave basis sets
    journal, February 2019

    Pervasive Delocalisation Error Causes Spurious Proton Transfer in Organic Acid-Base Co-Crystals
    journal, October 2018

    • LeBlanc, Luc M.; Dale, Stephen G.; Taylor, Christopher R.
    • Angewandte Chemie International Edition, Vol. 57, Issue 45
    • DOI: 10.1002/anie.201809381

    Coupling between oxygen redox and cation migration explains unusual electrochemistry in lithium-rich layered oxides
    journal, December 2017

    Density-functional description of alkalides: introducing the alkalide state
    journal, January 2018

    • Dale, Stephen G.; Becke, Axel D.; Johnson, Erin R.
    • Physical Chemistry Chemical Physics, Vol. 20, Issue 41
    • DOI: 10.1039/c8cp04014a

    Advanced capabilities for materials modelling with Quantum ESPRESSO
    journal, October 2017

    • Giannozzi, P.; Andreussi, O.; Brumme, T.
    • Journal of Physics: Condensed Matter, Vol. 29, Issue 46
    • DOI: 10.1088/1361-648x/aa8f79

    Hybrid DFT investigation of the energetics of Mg ion diffusion in α-MoO 3
    journal, January 2018

    • Barnes, Taylor A.; Wan, Liwen F.; Kent, Paul R. C.
    • Physical Chemistry Chemical Physics, Vol. 20, Issue 38
    • DOI: 10.1039/c8cp05511d

    Advanced capabilities for materials modelling with Quantum ESPRESSO
    text, January 2017

    Advanced capabilities for materials modelling with Quantum ESPRESSO
    text, January 2017

    Fast hybrid density-functional computations using plane-wave basis sets
    preprint, January 2018

    Coupling between oxygen redox and cation migration explains unusual electrochemistry in lithium-rich layered oxides
    journal, December 2017

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