Uncertainty quantification for predictions of atomistic neural networks.

The value of uncertainty quantification on predictions for trained neural networks (NNs) on quantum chemical reference data is quantitatively explored. For this, the architecture of the PhysNet NN was suitably modified and the resulting model (PhysNet-DER) was evaluated with different metrics to quantify its calibration, the quality of its predictions, and whether prediction error and the predicted uncertainty can be correlated. Training on the QM9 database and evaluating data in the test set within and outside the distribution indicate that error and uncertainty are not linearly related.