TY - JOUR

T1 - Coupled cluster theory on modern heterogeneous supercomputers

AU - Corzo, Hector H.

AU - Hillers-Bendtsen, Andreas Erbs

AU - Barnes, Ashleigh

AU - Zamani, Abdulrahman Y.

AU - Pawłowski, Filip

AU - Olsen, Jeppe

AU - Jørgensen, Poul

AU - Mikkelsen, Kurt V.

AU - Bykov, Dmytro

N1 - Correction: https://doi.org/10.3389/fchem.2023.1256510 Publisher Copyright: Copyright © 2023 Corzo, Hillers-Bendtsen, Barnes, Zamani, Pawłowski, Olsen, Jørgensen, Mikkelsen and Bykov.

PY - 2023

Y1 - 2023

N2 - This study examines the computational challenges in elucidating intricate chemical systems, particularly through ab-initio methodologies. This work highlights the Divide-Expand-Consolidate (DEC) approach for coupled cluster (CC) theory—a linear-scaling, massively parallel framework—as a viable solution. Detailed scrutiny of the DEC framework reveals its extensive applicability for large chemical systems, yet it also acknowledges inherent limitations. To mitigate these constraints, the cluster perturbation theory is presented as an effective remedy. Attention is then directed towards the CPS (D-3) model, explicitly derived from a CC singles parent and a doubles auxiliary excitation space, for computing excitation energies. The reviewed new algorithms for the CPS (D-3) method efficiently capitalize on multiple nodes and graphical processing units, expediting heavy tensor contractions. As a result, CPS (D-3) emerges as a scalable, rapid, and precise solution for computing molecular properties in large molecular systems, marking it an efficient contender to conventional CC models.

AB - This study examines the computational challenges in elucidating intricate chemical systems, particularly through ab-initio methodologies. This work highlights the Divide-Expand-Consolidate (DEC) approach for coupled cluster (CC) theory—a linear-scaling, massively parallel framework—as a viable solution. Detailed scrutiny of the DEC framework reveals its extensive applicability for large chemical systems, yet it also acknowledges inherent limitations. To mitigate these constraints, the cluster perturbation theory is presented as an effective remedy. Attention is then directed towards the CPS (D-3) model, explicitly derived from a CC singles parent and a doubles auxiliary excitation space, for computing excitation energies. The reviewed new algorithms for the CPS (D-3) method efficiently capitalize on multiple nodes and graphical processing units, expediting heavy tensor contractions. As a result, CPS (D-3) emerges as a scalable, rapid, and precise solution for computing molecular properties in large molecular systems, marking it an efficient contender to conventional CC models.

KW - cluster perturbation theory

KW - coupled cluster theory

KW - deoxyribonucleic acid

KW - divide-expand-consolidate coupled cluster framework

KW - excitation energies

KW - tetrahydrocannabinol

U2 - 10.3389/fchem.2023.1154526

DO - 10.3389/fchem.2023.1154526

M3 - Journal article

C2 - 37388945

AN - SCOPUS:85163727930

VL - 11

JO - Frontiers in Chemistry

JF - Frontiers in Chemistry

SN - 2296-2646

M1 - 1154526

ER -