Implementation of relativistic coupled cluster theory for massively parallel GPU-accelerated computing architectures

Abstract

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.

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Cited by in corpus (14)

• Implementation of relativistic coupled cluster theory for massively parallel GPU-accelerated computing architectures
• Towards Pair Atomic Density Fitting for Correlation Energies with Benchmark Accuracy
• Distributed Memory, GPU Accelerated Fock Construction for Hybrid, Gaussian Basis Density Functional Theory
• A lower scaling four-component relativistic coupled cluster method based on natural spinors
• Towards highly accurate calculations of parity violation in chiral molecules: relativistic coupled-cluster theory including QED-effects
• Assessing MP2 frozen natural orbitals in relativistic correlated electronic structure calculations
• Formulation and Implementation of Frequency-Dependent Linear Response Properties with Relativistic Coupled Cluster Theory for GPU-accelerated Computer Architectures
• Relativistic Exact Two-Component Coupled-Cluster Study of Molecular Sensitivity Factors for Nuclear Schiff Moments
• Electroweak Nuclear Properties from Single Molecular Ions in a Penning Trap
• Generating coupled cluster code for modern distributed memory tensor software
• Shifting sands of hardware and software in exascale quantum mechanical simulations
• Relativistic atomic structure calculations in support of spectroscopy
• The performance of approximate equation of motion coupled cluster for valence and core states of heavy element systems
• On the rank-reduced relativistic coupled cluster method