Multi-Fidelity Training Reshapes Uncertainty Decomposition in Atomistic Models

Overview & Synopsis

Multi-fidelity training, which combines abundant low-fidelity data with scarce high-fidelity labels, is increasingly common in atomistic modeling, but its effect on predictive uncertainty remains largely unexplored. We investigate this question using deep ensembles of mean-variance MACE models trained on ANI-1x, contrasting high-fidelity training from scratch with low-fidelity pretraining followed by fine-tuning. We characterize aleatoric, epistemic, and total uncertainty throughout training and under two distribution shifts: unseen molecular systems and higher-energy configurations. We find that pretraining reduces prediction error and improves uncertainty-based ranking across all test sets, but does not yield well-calibrated predictive variances; calibration deteriorates more severely under energy extrapolation. Training-dynamics analysis localizes most of this calibration degradation to high-fidelity optimization, during which the learned aleatoric variance becomes overconfident on held-out data. Moreover, multi-fidelity fine-tuning produces a more effective uncertainty-based acquisition function than high-fidelity training from scratch. These findings show that uncertainty ranking and calibration capture distinct properties and must be assessed separately in multi-fidelity atomistic models, especially under extrapolation.