TY - JOUR

T1 - Massively parallel GPU enabled third-order cluster perturbation excitation energies for cost-effective large scale excitation energy calculations

AU - Hillers-Bendtsen, Andreas Erbs

AU - Bykov, Dmytro

AU - Barnes, Ashleigh

AU - Liakh, Dmitry

AU - Corzo, Hector H.

AU - Olsen, Jeppe

AU - Jørgensen, Poul

AU - Mikkelsen, Kurt V.

N1 - Funding Information: This research used resources from the Oak Ridge Leadership Computing Facility, which is a DOE Office of Science User Facility supported under Contract No. DEAC05-00OR22725. A.E.H.B. and K.V.M. acknowledge the Danish Council for Independent Research (Grant No. DFF-0136-00081B) and the European Union’s Horizon 2020 Framework Program under Grant Agreement No. 951801 for financial support. Funding Information: Notice: This manuscript has been authored by UT-Battelle, LLC under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy. The publisher, by accepting the article for publication, acknowledges that the U.S. Government retains a non-exclusive, paid up, irrevocable, world-wide license to publish or reproduce the published form of the manuscript, or allow others to do so, for U.S. Government purposes. The DOE will provide public access to these results in accordance with the DOE Public Access Plan ( http://energy.gov/downloads/doe-public-access-plan ). Publisher Copyright: © 2023 Author(s).

PY - 2023

Y1 - 2023

N2 - We present here a massively parallel implementation of the recently developed CPS(D-3) excitation energy model that is based on cluster perturbation theory. The new algorithm extends the one developed in Baudin et al. [J. Chem. Phys., 150, 134110 (2019)] to leverage multiple nodes and utilize graphical processing units for the acceleration of heavy tensor contractions. Furthermore, we show that the extended algorithm scales efficiently with increasing amounts of computational resources and that the developed code enables CPS(D-3) excitation energy calculations on large molecular systems with a low time-to-solution. More specifically, calculations on systems with over 100 atoms and 1000 basis functions are possible in a few hours of wall clock time. This establishes CPS(D-3) excitation energies as a computationally efficient alternative to those obtained from the coupled-cluster singles and doubles model.

AB - We present here a massively parallel implementation of the recently developed CPS(D-3) excitation energy model that is based on cluster perturbation theory. The new algorithm extends the one developed in Baudin et al. [J. Chem. Phys., 150, 134110 (2019)] to leverage multiple nodes and utilize graphical processing units for the acceleration of heavy tensor contractions. Furthermore, we show that the extended algorithm scales efficiently with increasing amounts of computational resources and that the developed code enables CPS(D-3) excitation energy calculations on large molecular systems with a low time-to-solution. More specifically, calculations on systems with over 100 atoms and 1000 basis functions are possible in a few hours of wall clock time. This establishes CPS(D-3) excitation energies as a computationally efficient alternative to those obtained from the coupled-cluster singles and doubles model.

U2 - 10.1063/5.0142780

DO - 10.1063/5.0142780

M3 - Journal article

C2 - 37061462

AN - SCOPUS:85152566664

VL - 158

JO - The Journal of Chemical Physics

JF - The Journal of Chemical Physics

SN - 0021-9606

IS - 14

M1 - 144111

ER -