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Main Authors: Zaghen, Olga, Zhdanov, Maksim, Coscia, Dario, Wessels, David R., Bekkers, Erik J.
Format: Preprint
Published: 2026
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Online Access:https://arxiv.org/abs/2605.19939
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author Zaghen, Olga
Zhdanov, Maksim
Coscia, Dario
Wessels, David R.
Bekkers, Erik J.
author_facet Zaghen, Olga
Zhdanov, Maksim
Coscia, Dario
Wessels, David R.
Bekkers, Erik J.
contents Machine Learning Interatomic Potentials (MLIPs) achieve near ab initio accuracy at a fraction of the cost of quantum-mechanical simulations, yet they remain prone to silent failures on out-of-distribution configurations, making principled uncertainty quantification (UQ) essential for error-aware simulations and active learning. Existing non-ensemble UQ methods for MLIPs rely either on variational inference or on parametric distributional assumptions, both of which add architectural complexity and hyper-parameters that must be tuned per task. Inspired by recent advances in probabilistic weather forecasting, we propose a simpler alternative: turn a deterministic MLIP into a probabilistic one through learned functional perturbations and finetune it end-to-end with the Continuous Ranked Probability Score (CRPS), a proper scoring rule. We validate the approach with an equivariant GNN (P-EGNN) trained from scratch and by finetuning the foundation model the Orb-v3 for silica. On the N-body charged particle benchmark, P-EGNN improves CRPS over the state-of-the-art Bayesian MLIP method BLIP by 19-32% across all training sizes; on silica, P-Orb raises the Spearman correlation between predicted uncertainty and actual error from 0.75 (BLIP-Orb) to 0.84.
format Preprint
id arxiv_https___arxiv_org_abs_2605_19939
institution arXiv
publishDate 2026
record_format arxiv
spellingShingle Uncertainty-aware Machine Learning Interatomic Potentials via Learned Functional Perturbations
Zaghen, Olga
Zhdanov, Maksim
Coscia, Dario
Wessels, David R.
Bekkers, Erik J.
Computational Engineering, Finance, and Science
Machine Learning Interatomic Potentials (MLIPs) achieve near ab initio accuracy at a fraction of the cost of quantum-mechanical simulations, yet they remain prone to silent failures on out-of-distribution configurations, making principled uncertainty quantification (UQ) essential for error-aware simulations and active learning. Existing non-ensemble UQ methods for MLIPs rely either on variational inference or on parametric distributional assumptions, both of which add architectural complexity and hyper-parameters that must be tuned per task. Inspired by recent advances in probabilistic weather forecasting, we propose a simpler alternative: turn a deterministic MLIP into a probabilistic one through learned functional perturbations and finetune it end-to-end with the Continuous Ranked Probability Score (CRPS), a proper scoring rule. We validate the approach with an equivariant GNN (P-EGNN) trained from scratch and by finetuning the foundation model the Orb-v3 for silica. On the N-body charged particle benchmark, P-EGNN improves CRPS over the state-of-the-art Bayesian MLIP method BLIP by 19-32% across all training sizes; on silica, P-Orb raises the Spearman correlation between predicted uncertainty and actual error from 0.75 (BLIP-Orb) to 0.84.
title Uncertainty-aware Machine Learning Interatomic Potentials via Learned Functional Perturbations
topic Computational Engineering, Finance, and Science
url https://arxiv.org/abs/2605.19939