Hybrid Data‐Driven Discovery of High‐Performance Silver Selenide‐Based Thermoelectric Composites

Abstract Optimizing material compositions often enhances thermoelectric performances. However, the large selection of possible base elements and dopants results in a vast composition design space that is too large to systematically search using solely domain knowledge. To address this challenge, a hybrid data‐driven strategy that integrates Bayesian optimization (BO) and Gaussian process regression (GPR) is proposed to optimize the composition of five elements (Ag, Se, S, Cu, and Te) in AgSe‐based thermoelectric materials. Data is collected from the literature to provide prior knowledge for the initial GPR model, which is updated by actively collected experimental data during the iteration between BO and experiments. Within seven iterations, the optimized AgSe‐based materials prepared using a simple high‐throughput ink mixing and blade coating method deliver a high power factor of 2100 µW m⁻¹ K⁻², which is a 75% improvement from the baseline composite (nominal composition of Ag₂Se₁). The success of this study provides opportunities to generalize the demonstrated active machine learning technique to accelerate the development and optimization of a wide range of material systems with reduced experimental trials.