Breaking the Million-Electron and 1 EFLOP/s Barriers: Biomolecular-Scale Ab Initio Molecular Dynamics Using MP2 Potentials

TL;DR

This paper introduces a GPU-accelerated method combining molecular fragmentation and MP2 perturbation theory, enabling biomolecular-scale ab initio molecular dynamics at unprecedented scale and quantum accuracy, breaking previous computational barriers.

Contribution

The study presents a novel approach that combines fragmentation, MP2 theory, and GPU optimization to perform large-scale AIMD simulations at wave-function accuracy.

Findings

Achieved 59% of Frontier's peak performance (1006.7 PFLOP/s)

Simulated systems with over a million electrons

Surpassed 1 EFLOP/s computational barrier

Abstract

The accurate simulation of complex biochemical phenomena has historically been hampered by the computational requirements of high-fidelity molecular-modeling techniques. Quantum mechanical methods, such as ab initio wave-function (WF) theory, deliver the desired accuracy, but have impractical scaling for modelling biosystems with thousands of atoms. Combining molecular fragmentation with MP2 perturbation theory, this study presents an innovative approach that enables biomolecular-scale ab initio molecular dynamics (AIMD) simulations at WF theory level. Leveraging the resolution-of-the-identity approximation for Hartree-Fock and MP2 gradients, our approach eliminates computationally intensive four-center integrals and their gradients, while achieving near-peak performance on modern GPU architectures. The introduction of asynchronous time steps minimizes time step latency, overlapping computational phases and effectively mitigating load imbalances. Utilizing up to 9,400 nodes of Frontier and achieving 59% (1006.7 PFLOP/s) of its double-precision floating-point peak, our method enables us to break the million-electron and 1 EFLOP/s barriers for AIMD simulations with quantum accuracy.