Designing functional molecules and advanced materials requires complex interdependent design choices: tuning continuous process parameters such as temperatures or flow rates, while simultaneously selecting categorical variables like catalysts or solvents. To date, the development of data-driven experiment planning strategies for autonomous experimentation has largely focused on continuous process parameters despite the urge to devise efficient strategies for the selection of categorical variables to substantially accelerate scientific discovery. We introduce Gryffin, as a general purpose optimization framework for the autonomous selection of categorical variables driven by expert knowledge. Gryffin augments Bayesian optimization with kernel density estimation using smooth approximations to categorical distributions. Leveraging domain knowledge from physicochemical descriptors to characterize categorical options, Gryffin can significantly accelerate the search for promising molecules and materials. Gryffin can further highlight relevant correlations between the provided descriptors to inspire physical insights and foster scientific intuition. In addition to comprehensive benchmarks, we demonstrate the capabilities and performance of Gryffin on three examples in materials science and chemistry: (i) the discovery of non-fullerene acceptors for organic solar cells, (ii) the design of hybrid organic-inorganic perovskites for light-harvesting, and (iii) the identification of ligands and process parameters for Suzuki-Miyaura reactions. Our observations suggest that Gryffin, in its simplest form without descriptors, constitutes a competitive categorical optimizer compared to state-of-the-art approaches. However, when leveraging domain knowledge provided via descriptors, Gryffin can optimize at considerable higher rates and refine this domain knowledge to spark scientific understanding.

本研究介绍了Gryffin，一种基于专家知识驱动的分类变量自主实验选择优化框架，它能够利用物理化学描述符，显著加速寻找有前途的分子和材料，并在化学和材料科学中的三个实例中展示了其性能和功能。

Gryffin: 一种基于专家知识的分类变量贝叶斯优化算法