论文标题
贝叶斯优化具有化学应用的已知实验和设计约束
Bayesian optimization with known experimental and design constraints for chemistry applications
论文作者
论文摘要
在实验科学中探索了由机器学习驱动的优化策略,例如贝叶斯优化,作为传统实验设计的有效替代方法。当与自动实验室硬件和高性能计算结合使用时,这些策略可以实现下一代平台进行自主实验。但是,由于缺乏针对化学研究的独特要求而定制的灵活软件和算法,这些方法的实际应用受到了阻碍。这样的方面之一是优化化学过程或方案以及在设计功能分子或材料时可访问的化学空间时,在实验条件下普遍存在约束。尽管这些约束中的许多都是先验的,但它们可以相互依存,非线性,并导致非紧凑型优化域。在这项工作中,我们扩展了实验规划算法腓尼和格兰芬,以便他们可以通过直观且灵活的界面处理任意的已知约束。我们将这些扩展的算法基准在具有多种约束的连续和离散测试功能上,表明它们的灵活性和鲁棒性。此外,我们在两个模拟化学研究方案中说明了它们的实际实用性:在约束流条件下,O-二甲基甲苯基杆骨加合物的合成的优化,以及在合成可访问性约束下对流量电池的氧化还原活性分子的设计。开发的工具构成了一种简单但多才多艺的策略,可通过已知的实验约束来实现基于模型的优化,这有助于其作为科学发现自主平台的核心组成部分。
Optimization strategies driven by machine learning, such as Bayesian optimization, are being explored across experimental sciences as an efficient alternative to traditional design of experiment. When combined with automated laboratory hardware and high-performance computing, these strategies enable next-generation platforms for autonomous experimentation. However, the practical application of these approaches is hampered by a lack of flexible software and algorithms tailored to the unique requirements of chemical research. One such aspect is the pervasive presence of constraints in the experimental conditions when optimizing chemical processes or protocols, and in the chemical space that is accessible when designing functional molecules or materials. Although many of these constraints are known a priori, they can be interdependent, non-linear, and result in non-compact optimization domains. In this work, we extend our experiment planning algorithms Phoenics and Gryffin such that they can handle arbitrary known constraints via an intuitive and flexible interface. We benchmark these extended algorithms on continuous and discrete test functions with a diverse set of constraints, demonstrating their flexibility and robustness. In addition, we illustrate their practical utility in two simulated chemical research scenarios: the optimization of the synthesis of o-xylenyl Buckminsterfullerene adducts under constrained flow conditions, and the design of redox active molecules for flow batteries under synthetic accessibility constraints. The tools developed constitute a simple, yet versatile strategy to enable model-based optimization with known experimental constraints, contributing to its applicability as a core component of autonomous platforms for scientific discovery.