Diagnostic Accuracy Is Not Deployment Value: Decision-Aligned Reliability Evaluation for Foundation MLIPs in Materials Discovery
Abstract
In AI-guided materials discovery, machine-learning models increasingly decide which candidate materials should receive expensive first-principles or experimental evaluation. Standard reliability metrics such as uncertainty, calibration, novelty, and ranking accuracy evaluate properties of the predictions, but success on these metrics does not necessarily imply a better downstream screening decision. We study this mismatch for foundation machine-learned interatomic potentials (MACE-MP, CHGNet, Orb V3) used to rank candidate crystal structures before DFT verification. We evaluate three representative reliability interventions (novelty detection, sparse DFT calibration, and chemistry-level ranking audits) using a deployment objective that measures how much DFT can be avoided while maintaining a required recall of near-hull candidates. Across all three, a reliability signal can succeed on its immediate target without improving the final screening decision: novelty detects distribution shift but weakly ranks failure severity; calibration can improve pooled ranking metrics while leaving screening unchanged or degrading it; and sparse audits identify MLIP–chemistry combinations with poor ranking reliability without yielding a robustly beneficial routing policy. A two-oracle analysis further shows that the source of failure depends on the screening decision itself: under formation-energy screening, even perfect knowledge of average ranking reliability can select the wrong model, whereas under a hull-aligned scoring variant that oracle target becomes decision-aligned but finite-budget audits still fail to realize the value. Reliability should be evaluated relative to the decision it supports: the relevant question is not whether a model is uncertain or inaccurate, but whether acquiring and acting on additional information will improve the final discovery decision enough to justify its cost.