AIQM2: Organic Reaction Simulations Beyond DFT

Abstract

Density functional theory (DFT) is the workhorse of reaction simulations, but it often suffers from either prohibitive cost or insufficient accuracy. In this work, we report AIQM2—the universal AI-enhanced QM Method 2—as the first method that enables fast and accurate large-scale organic reaction simulations for practically relevant system sizes and time scales beyond what is possible with DFT. This breakthrough is based on the high speed of AIQM2, which is orders of magnitude faster than common DFT, while its accuracy in reaction energies, transition state optimizations, and barrier heights is at least at the level of DFT and often approaches the gold-standard coupled cluster accuracy. AIQM2 can be used out of the box without any further retraining. Compared to pure machine learning potentials, AIQM2 possesses high transferability and robustness in simulations without catastrophic breakdowns. We showcase the superiority of AIQM2 compared to traditional DFT by performing an extensive reaction dynamics study overnight and revising the mechanism and product distribution reported in the previous investigation of the bifurcating pericyclic reaction.