Learned Force Fields Are Ready For Ground State Catalyst Discovery

by   Michael Schaarschmidt, et al.

We present evidence that learned density functional theory (“DFT”) force fields are ready for ground state catalyst discovery. Our key finding is that relaxation using forces from a learned potential yields structures with similar or lower energy to those relaxed using the RPBE functional in over 50% of evaluated systems, despite the fact that the predicted forces differ significantly from the ground truth. This has the surprising implication that learned potentials may be ready for replacing DFT in challenging catalytic systems such as those found in the Open Catalyst 2020 dataset. Furthermore, we show that a force field trained on a locally harmonic energy surface with the same minima as a target DFT energy is also able to find lower or similar energy structures in over 50% of cases. This “Easy Potential” converges in fewer steps than a standard model trained on true energies and forces, which further accelerates calculations. Its success illustrates a key point: learned potentials can locate energy minima even when the model has high force errors. The main requirement for structure optimisation is simply that the learned potential has the correct minima. Since learned potentials are fast and scale linearly with system size, our results open the possibility of quickly finding ground states for large systems.


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