James E. Saal

Qian Du, Mark M. Sullivan, James E. Saal et al.

This study presents an iterative AI-guided workflow that accelerates graphite-based anode development by improving both formulation feasibility and process robustness. Sequential learning via AI/ML-guided multiobjective inverse design for anode optimization was implemented using the Citrine Platform. Starting from a noisy, incomplete dataset, the Citrine Platform was used to generate early surrogate models, which despite low predictive certainty highlighted missing process constraints. By iteratively adding feasibility labels and boundary condition failures, the workflow rapidly converged toward manufacturable, higher-performing formulations. Fabrication reliability improved from frequent process failures to 100% successful cell production, while the fraction of cells delivering $\geq$ 350 mAh g$^{-1}$ increased from 28.4% to 84.8%, with capacity retention rising from 42.1% to 97.3%. These results demonstrate that structured, feedback-driven AI workflows can transform imperfect industrial data into actionable guidance, enabling faster, more reproducible optimization of battery electrode manufacturing.

Eric S. Muckley, James E. Saal, Bryce Meredig et al.

Data-driven models are central to scientific discovery. In efforts to achieve state-of-the-art model accuracy, researchers are employing increasingly complex machine learning algorithms that often outperform simple regressions in interpolative settings (e.g. random k-fold cross-validation) but suffer from poor extrapolation performance, portability, and human interpretability, which limits their potential for facilitating novel scientific insight. Here we examine the trade-off between model performance and interpretability across a broad range of science and engineering problems with an emphasis on materials science datasets. We compare the performance of black box random forest and neural network machine learning algorithms to that of single-feature linear regressions which are fitted using interpretable input features discovered by a simple random search algorithm. For interpolation problems, the average prediction errors of linear regressions were twice as high as those of black box models. Remarkably, when prediction tasks required extrapolation, linear models yielded average error only 5% higher than that of black box models, and outperformed black box models in roughly 40% of the tested prediction tasks, which suggests that they may be desirable over complex algorithms in many extrapolation problems because of their superior interpretability, computational overhead, and ease of use. The results challenge the common assumption that extrapolative models for scientific machine learning are constrained by an inherent trade-off between performance and interpretability.

Sarah I. Allec, Xiaonan Lu, Daniel R. Cassar et al.

Glasses form the basis of many modern applications and also hold great potential for future medical and environmental applications. However, their structural complexity and large composition space make design and optimization challenging for certain applications. Of particular importance for glass processing is an estimate of a given composition's glass-forming ability (GFA). However, there remain many open questions regarding the physical mechanisms of glass formation, especially in oxide glasses. It is apparent that a proxy for GFA would be highly useful in glass processing and design, but identifying such a surrogate property has proven itself to be difficult. Here, we explore the application of an open-source pre-trained NN model, GlassNet, that can predict the characteristic temperatures necessary to compute glass stability (GS) and assess the feasibility of using these physics-informed ML (PIML)-predicted GS parameters to estimate GFA. In doing so, we track the uncertainties at each step of the computation - from the original ML prediction errors, to the compounding of errors during GS estimation, and finally to the final estimation of GFA. While GlassNet exhibits reasonable accuracy on all individual properties, we observe a large compounding of error in the combination of these individual predictions for the prediction of GS, finding that random forest models offer similar accuracy to GlassNet. We also breakdown the ML performance on different glass families and find that the error in GS prediction is correlated with the error in crystallization peak temperature prediction. Lastly, we utilize this finding to assess the relationship between top-performing GS parameters and GFA for two ternary glass systems: sodium borosilicate and sodium iron phosphate glasses. We conclude that to obtain true ML predictive capability of GFA, significantly more data needs to be collected.