Hierarchical automation of scanning probe microscopy through agentic orchestration and algorithmic control
Rapid advances in agentic artificial intelligence enable scientific systems to interpret open-ended objectives, combine heterogeneous information, invoke specialized tools, and revise experimental strategies as evidence accumulates. However, physical experimentation also contains many tasks for which agentic reasoning provides little advantage and can reduce reliability. Quantitative analysis, optimization, spatial targeting, validation, and instrument execution are often better posed as deterministic or algorithmic operations with explicit objectives and verifiable outputs. Here, we introduce a hierarchical architecture for autonomous experimentation that separates these roles. Agentic components interpret scientific intent, construct task-dependent experimental representations, evaluate accumulated evidence, and select high-level actions, whereas deterministic algorithms perform numerical analysis, coordinate selection, validation, and physical execution. We implement this architecture in piezoresponse force microscopy. Starting from a broad scientific question concerning the relation between local domain structure and polarization switching, the system constructs spatial descriptors from multichannel imaging, selects and analyzes local hysteresis measurements, adapts the spectroscopy waveform, and terminates the experiment when additional measurements cease to provide new evidence. The autonomous trajectory also identifies a confounding relationship between polarization state and domain-wall proximity and recognizes that the requested contrast is not independently represented within the available field of view. These results demonstrate a route toward scientific autonomy in which agents determine what evidence is required while algorithms determine how that evidence is acquired reproducibly and within validated physical constraints.