Robert Black

Ali Jaberi, Yonatan Kurniawan, Robert Black et al.

This paper introduces AutoREC, an open-source Python package for developing reinforcement learning (RL) agents to automatically generate equivalent circuit models (ECMs) from electrochemical impedance spectroscopy (EIS) data. While ECMs are a standard framework for interpreting EIS data, traditional identification is typically based on manual trial-and-error, which requires domain experts and limits scalability, particularly in autonomous experimental pipelines such as self-driving laboratories. AutoREC addresses this challenge by formulating ECM construction as a sequential decision-making problem within a Markov Decision Process framework. It implements a Double Deep Q-Network with prioritized experience replay, along with a dedicated dead-loop mitigation strategy, to efficiently explore a complex action space for circuit generation. To demonstrate the capabilities of the platform, we trained an RL agent using AutoREC and evaluated its strengths and limitations across diverse datasets, while also discussing possible strategies to mitigate these limitations in future agent designs. The trained agent achieved a success rate exceeding $99.6\%$ on synthetic datasets and demonstrated strong generalization to unseen experimental EIS data from batteries, corrosion, oxygen evolution reaction, and CO$_2$ reduction systems. These results position AutoREC as a promising platform for adaptive and data-driven ECM generation, with potential for integration into automated electrochemical workflows.

Ali Jaberi, Amin Sadeghi, Runze Zhang et al.

Electrochemical impedance spectroscopy (EIS) data is typically modeled using an equivalent circuit model (ECM), with parameters obtained by minimizing a loss function via nonlinear least squares fitting. This paper introduces two new loss functions, log-B and log-BW, derived from the Bode representation of EIS. Using a large dataset of generated EIS data, the performance of proposed loss functions was evaluated alongside existing ones in terms of R2 scores, chi-squared, computational efficiency, and the mean absolute percentage error (MAPE) between the predicted component values and the original values. Statistical comparisons revealed that the choice of loss function impacts convergence, computational efficiency, quality of fit, and MAPE. Our analysis showed that X2 loss function (squared sum of residuals with proportional weighting) achieved the highest performance across multiple quality of fit metrics, making it the preferred choice when the quality of fit is the primary goal. On the other hand, log-B offered a slightly lower quality of fit while being approximately 1.4 times faster and producing lower MAPE for most circuit components, making log-B as a strong alternative. This is a critical factor for large-scale least squares fitting in data-driven applications, such as training machine learning models on extensive datasets or iterations.

Qiuyu Shi, Kangming Li, Yao Fehlis et al.

Self-driving laboratories (SDLs) have shown promise to accelerate materials discovery by integrating machine learning with automated experimental platforms. However, errors in the capture of input parameters may corrupt the features used to model system performance, compromising current and future campaigns. This study develops an automated workflow to systematically detect noisy features, determine sample-feature pairings that can be corrected, and finally recover the correct feature values. A systematic study is then performed to examine how dataset size, noise intensity, and feature value distribution affect both the detectability and recoverability of noisy features. In general, high-intensity noise and large training datasets are conducive to the detection and correction of noisy features. Low-intensity noise reduces detection and recovery but can be compensated for by larger clean training data sets. Detection and correction results vary between features with continuous and dispersed feature distributions showing greater recoverability compared to features with discrete or narrow distributions. This systematic study not only demonstrates a model agnostic framework for rational data recovery in the presence of noise, limited data, and differing feature distributions but also provides a tangible benchmark of kNN imputation in materials data sets. Ultimately, it aims to enhance data quality and experimental precision in automated materials discovery.

Yutong Liu, Mehrad Ansari, Robert Black et al.

Machine learning and high-throughput experimentation have greatly accelerated the discovery of mixed metal oxide catalysts by leveraging their compositional flexibility. However, the lack of established synthesis routes for solid-state materials remains a significant challenge in inorganic chemistry. An interpretable machine learning model is therefore essential, as it provides insights into the key factors governing phase formation. Here, we focus on the formation of single-phase Fe$_2$(ZnCo)O$_4$, synthesized via a high-throughput co-precipitation method. We combined a kernel classification model with a novel application of global SHAP analysis to pinpoint the experimental features most critical to single phase synthesizability by interpreting the contributions of each feature. Global SHAP analysis reveals that precursor and precipitating agent contributions to single-phase spinel formation align closely with established crystal growth theories. These results not only underscore the importance of interpretable machine learning in refining synthesis protocols but also establish a framework for data-informed experimental design in inorganic synthesis.