Autonomous battery research: Principles of heuristic operando experimentation
Traditional in situ battery characterization methods struggle to reliably capture stochastic, transient failure events such as dendrite initiation. This work proposes a heuristic in situ experimental framework that integrates physics-informed digital twins with AI agents to actively guide multimodal beamline instrumentation toward mechanistically critical precursors. Departing from conventional uncertainty-driven active learning, the approach innovatively employs entropy-based metrics to quantify scientific information gain, thereby enhancing experimental efficiency and data value while adhering to FAIR data principles. The method effectively mitigates beam-induced damage and data redundancy, successfully capturing transient precursor phenomena overlooked by conventional techniques, and establishes a new paradigm for building trustworthy autonomous battery laboratories.