Transition1x -- a Dataset for Building Generalizable Reactive Machine Learning Potentials
This provides a new benchmark for developing generalizable ML force fields for reactive systems, addressing a domain-specific bottleneck in computational chemistry.
The authors tackled the problem of machine learning models failing as surrogate potentials for reaction barrier search due to lack of training data in transition state regions, by presenting the Transition1x dataset with 9.6 million DFT calculations and showing that models cannot learn these features from existing datasets.
Machine Learning (ML) models have, in contrast to their usefulness in molecular dynamics studies, had limited success as surrogate potentials for reaction barrier search. It is due to the scarcity of training data in relevant transition state regions of chemical space. Currently, available datasets for training ML models on small molecular systems almost exclusively contain configurations at or near equilibrium. In this work, we present the dataset Transition1x containing 9.6 million Density Functional Theory (DFT) calculations of forces and energies of molecular configurations on and around reaction pathways at the wB97x/6-31G(d) level of theory. The data was generated by running Nudged Elastic Band (NEB) calculations with DFT on 10k reactions while saving intermediate calculations. We train state-of-the-art equivariant graph message-passing neural network models on Transition1x and cross-validate on the popular ANI1x and QM9 datasets. We show that ML models cannot learn features in transition-state regions solely by training on hitherto popular benchmark datasets. Transition1x is a new challenging benchmark that will provide an important step towards developing next-generation ML force fields that also work far away from equilibrium configurations and reactive systems.