AutoSAS: a new human-aside-the-loop paradigm for automated SAS fitting for high throughput and autonomous experimentation

TL;DR

AutoSAS introduces a human-in-the-loop framework for automated scattering data analysis, combining expert models, high-throughput fitting, and information theory to improve structural characterization in autonomous experiments.

Contribution

It presents AutoSAS, an open-source tool that enhances autonomous scattering data analysis with model selection and structural insights, integrating human expertise with automation.

Findings

AutoSAS successfully classified and refined structures in complex formulations.

The best model selection method balanced fit quality and complexity.

AutoSAS identified a new structural transition boundary.

Abstract

The advancement of artificial-intelligence driven autonomous experiments demands physics-based modeling and decision-making processes, not only to improve the accuracy of the experimental trajectory but also to increase trust by allowing transparent human-machine collaboration. High-quality structural characterization techniques (e.g., X-ray, neutron, or static light scattering) are a particularly relevant example of this need: they provide invaluable information but are challenging to analyze without expert oversight. Here, we introduce AutoSAS, a novel framework for human-aside-the-loop automated data classification. AutoSAS leverages human-defined candidate models, high-throughput combinatorial fitting, and information-theoretic model selection to generate both classification results and quantitative structural descriptors. We implement AutoSAS in an open-source package designed for use with the Autonomous Formulation Laboratory (AFL) for X-ray and neutron scattering-based optimization of multicomponent liquid formulations. In a first application, we leveraged a set of expert defined candidate models to classify, refine the structure, and track transformations in a model injectable drug carrier system. We evaluated four model selection methods and benchmarked them against an optimized machine learning classifier and the best approach was one that balanced quality of the fit and complexity of the model. AutoSAS not only corroborated the critical micelle concentration boundary identified in previous experiments but also discovered a second structural transition boundary not identified by the previous methods. These results demonstrate the potential of AutoSAS to enhance autonomous experimental workflows by providing robust, interpretable model selection, paving the way for more reliable and insightful structural characterization in complex formulations.