Massive-parallel Implementation of the Resolution-of-Identity Coupled-cluster Approaches in the Numeric Atom-centered Orbital Framework for Molecular Systems

TL;DR

This paper introduces a highly scalable parallel implementation of the RI-CCSD(T) method within the FHI-aims package, enabling efficient and accurate quantum chemical calculations for large molecular systems on supercomputers.

Contribution

It develops a domain-based distributed-memory algorithm for RI-CCSD(T) that minimizes communication and disk storage, achieving excellent scaling on thousands of cores.

Findings

Achieves strong scaling up to over 10,000 cores.

Demonstrates competitive performance with state-of-the-art HPC packages.

Shows negligible numerical error from RI approximation.

Abstract

We present a massive-parallel implementation of the resolution-of-identity (RI) coupled-cluster approach that includes single, double and perturbatively triple excitations, namely RI-CCSD(T), in the FHI-aims package for molecular systems. A domain-based distributed-memory algorithm in the MPI/OpenMP hybrid framework has been designed to effectively utilize the memory bandwidth and significantly minimize the interconnect communication, particularly for the tensor contraction in the evaluation of the particle-particle ladder term. Our implementation features a rigorous avoidance of the on-the-fly disk storage and an excellent strong scaling up to 10,000 and more cores. Taking a set of molecules with different sizes, we demonstrate that the parallel performance of our CCSD(T) code is competitive with the CC implementations in state-of-the-art high-performance computing (HPC) computational chemistry packages. We also demonstrate that the numerical error due to the use of RI approximation in our RI-CCSD(T) is negligibly small. Together with the correlation-consistent numeric atom-centered orbital (NAO) basis sets, NAO-VCC-nZ, the method is applied to produce accurate theoretical reference data for 22 bio-oriented weak interactions (S22), 11 conformational energies of gaseous cysteine conformers (CYCONF), and 32 isomerization energies (ISO32).