The training dataset was assembled from ANI-1x , which contains energies and forces from 5 million density functional theory calculations for small molecules. A fixed validation dataset of 50,000 frames was held out by random sampling. Different splits of training were taken with sizes 10 n where n ∈ . Training datasets for TPE were assembled by randomly sampling 1,000 structures from molecular dynamics (MD) trajectories for each of the 10 molecules available in the revised MD-17 dataset, for a total of 10,000 training samples. A validation dataset of equal size was constructed from the remaining geometries. Revised MD-17 is an updated version of the MD-17 dataset, recomputed at the PBE/def2-SVP level of theory with strict convergence criteria to remove noise found in the original MD-17 dataset.