Implementation of Relativistic Coupled Cluster Theory for Massively Parallel GPU-Accelerated Computing Architectures

Johann V. Pototschnig*, Anastasios Papadopoulos*, Dmitry I. Lyakh, Michal Repisky, Loïc Halbert, André Severo Pereira Gomes*, Hans Jørgen Aa Jensen*, Lucas Visscher*

*Corresponding author for this work

Research output: Contribution to journalJournal articleResearchpeer-review


In this paper, we report reimplementation of the core algorithms of relativistic coupled cluster theory aimed at modern heterogeneous high-performance computational infrastructures. The code is designed for 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 the electronic structure are included from the outset. In the current work, we thereby focus on exact two-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 the starting point, but it 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.

Original languageEnglish
JournalJournal of Chemical theory and Computation
Issue number9
Pages (from-to)5509-5529
Publication statusPublished - 14. Sep 2021

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© 2021 The Authors. Published by American Chemical Society.


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