High-Performance Multi-GPU Analytic RI-MP2 Energy Gradients.

Abstract

This article presents a novel algorithm for the calculation of analytic energy gradients from second-order Møller-Plesset perturbation theory within the Resolution-of-the-Identity approximation (RI-MP2), which is designed to achieve high performance on clusters with multiple graphical processing units (GPUs). The algorithm uses GPUs for all major steps of the calculation, including integral generation, formation of all required intermediate tensors, solution of the Z-vector equation and gradient accumulation. The implementation in the EXtreme Scale Electronic Structure System (EXESS) software package includes a tailored, highly efficient, multistream scheduling system to hide CPU-GPU data transfer latencies and allows nodes with 8 A100 GPUs to operate at over 80% of theoretical peak floating-point performance. Comparative performance analysis shows a significant reduction in computational time relative to traditional multicore CPU-based methods, with our approach achieving up to a 95-fold speedup over the single-node performance of established software such as Q-Chem and ORCA. Additionally, we demonstrate that pairing our implementation with the molecular fragmentation framework in EXESS can drastically lower the computational scaling of RI-MP2 gradient calculations from quintic to subquadratic, enabling further substantial savings in runtime while retaining high numerical accuracy in the resulting gradients.