Real-time Equation-of-Motion Coupled-Cluster Cumulant Green's Function Method: Heterogeneous Parallel Implementation Based on the Tensor Algebra for Many-body Methods Infrastructure

TL;DR

This paper presents a scalable, GPU-accelerated implementation of the real-time equation-of-motion coupled-cluster cumulant Green's function method within the TAMM tensor infrastructure, enabling accurate spectral simulations for large molecules.

Contribution

The authors developed a fully complex algebra, massively parallel implementation of RT-EOM-CC within TAMM, supporting large-scale spectral calculations on heterogeneous GPU systems.

Findings

Achieved over 90% parallel efficiency up to 400 GPUs.

Successfully simulated core photo-emission spectra for molecules with hundreds of orbitals.

Results agree well with experimental ionization energies.

Abstract

We report the implementation of the real-time equation-of-motion coupled-cluster (RT-EOM-CC) cumulant Green's function method [J. Chem. Phys. 152, 174113 (2020)] within the Tensor Algebra for Many-body Methods (TAMM) infrastructure. TAMM is a massively parallel heterogeneous tensor library designed for utilizing forthcoming exascale computing resources. The two-body electron repulsion matrix elements are Cholesky-decomposed, and we imposed spin-explicit forms of the various operators when evaluating the tensor contractions. Unlike our previous real algebra Tensor Contraction Engine (TCE) implementation, the TAMM implementation supports fully complex algebra. The RT-EOM-CC singles (S) and doubles (D) time-dependent amplitudes are propagated using a first-order Adams--Moulton method. This new implementation shows excellent scalability tested up to 500 GPUs using the Zn-porphyrin molecule with 655 basis functions, with parallel efficiencies above 90\% up to 400 GPUs. The TAMM RT-EOM-CCSD was used to study core photo-emission spectra in the formaldehyde and ethyl trifluoroacetate (ESCA) molecules. Simulations of the latter involve as many as 71 occupied and 649 virtual orbitals. The relative quasiparticle ionization energies and overall spectral functions agree well with available experimental results.