1. Implementation of relativistic coupled cluster theory for massively parallel GPU-accelerated computing architectures
- Author
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Loïc Halbert, Michal Repisky, Hans Jørgen Aa. Jensen, Lucas Visscher, Anastasios Papadopoulos, Dmitry I. Lyakh, André Severo Pereira Gomes, Johann V. Pototschnig, Department of Chemistry and Pharmaceutical Sciences, Vrije Universiteit Amsterdam [Amsterdam] (VU), National Center for Computational Sciences, Oak Ridge National Laboratory, Hylleraas Centre for Quantum Molecular Sciences (Hylleraas), Department of Chemistry [Oslo], Faculty of Mathematics and Natural Sciences [Oslo], University of Oslo (UiO)-University of Oslo (UiO)-Faculty of Mathematics and Natural Sciences [Oslo], University of Oslo (UiO)-University of Oslo (UiO), Physico-Chimie Moléculaire Théorique (PCMT), Laboratoire de Physique des Lasers, Atomes et Molécules - UMR 8523 (PhLAM), Université de Lille-Centre National de la Recherche Scientifique (CNRS)-Université de Lille-Centre National de la Recherche Scientifique (CNRS), Department of Physics, Chemistry and Pharmacy, University of Southern Denmark, Campusvej 55, 5230 Odense, Denmark, Oak Ridge Leadership Computing Facility, which is a DOE Office of Science User Facility supported under ContractDE-AC05-00OR22725, French Ministry of Higher Education and Research, region Hauts de France council and European Regional Development Fund (ERDF) project CPER CLIMIBIO, French national supercomputing facilities (grants DARI A0070801859 and Joliot Curie grands challenges 2019 gch0417)., MESONM International Associated Laboratory (LAI) (ANR-16-IDEX-0004), Austrian Science Fund(FWF):J 4177-N36, Research Council of Norway through a Center of Excellence Grant (Grant No. 262695), ANR-11-LABX-0005,Cappa,Physiques et Chimie de l'Environnement Atmosphérique(2011), ANR-19-CE29-0019,CompRIXS,Calcul de la diffusion inélastique résonante de rayons X pour toute la classification périodique(2019), ANR-16-IDEX-0004,ULNE,ULNE(2016), University of Southern Denmark (SDU), Theoretical Chemistry, and AIMMS
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Computer science ,Dirac (software) ,FOS: Physical sciences ,010402 general chemistry ,01 natural sciences ,Article ,Field (computer science) ,Computational science ,Set (abstract data type) ,Software ,Physics - Chemical Physics ,0103 physical sciences ,Point (geometry) ,SDG 7 - Affordable and Clean Energy ,Physical and Theoretical Chemistry ,Massively parallel ,Chemical Physics (physics.chem-ph) ,010304 chemical physics ,business.industry ,0104 chemical sciences ,Computer Science Applications ,[CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry ,Coupled cluster ,[PHYS.PHYS.PHYS-CHEM-PH]Physics [physics]/Physics [physics]/Chemical Physics [physics.chem-ph] ,Relativistic quantum chemistry ,business - Abstract
International audience; In this paper, we report a reimplementation of the core algorithms of relativistic coupled cluster theory aimed at modern heterogeneous high-performance computational infrastructures. The code is designed for efficient parallel execution on many compute nodes with optional GPU coprocessing, accomplished via the new ExaTENSOR back end. The resulting ExaCorr module is primarily intended for calculations of molecules with one or more heavy elements, as relativistic effects on electronic structure are included from the outset. In the current work, we thereby focus on exact 2-component methods and demonstrate the accuracy and performance of the software. The module can be used as a stand-alone program requiring a set of molecular orbital coefficients as starting point, but is also interfaced to the DIRAC program that can be used to generate these. We therefore also briefly discuss an improvement of the parallel computing aspects of the relativistic self-consistent field algorithm of the DIRAC program.
- Published
- 2021
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