Generating $\pi$-Functional Molecules Using STGG+ with Active Learning

Abstract

Generating novel molecules with out-of-distribution properties is a major challenge in molecular discovery. While supervised learning methods generate high-quality molecules similar to those in a dataset, they struggle to generalize to out-of-distribution properties. Reinforcement learning can explore novel spaces but often conducts 'reward-hacking' and generates non-synthesizable molecules. In this work, we address this problem by integrating a state-of-the-art supervised learning method, STGG+, in an active learning loop. Our approach iteratively generates, evaluates, and fine-tunes STGG+ to continuously expand its knowledge. We apply this method to the design of organic $\pi$-functional materials, specifically two challenging tasks: 1) generating highly absorptive molecules characterized by a large oscillator strength and 2) designing absorptive molecules with reasonable oscillator strength in the near-infrared range. The generated molecules are validated and rationalized \textit{in-silico} with time-dependent density functional theory. Our results demonstrate that our method is highly effective in generating novel molecules with high oscillator strength, contrary to existing methods such as reinforcement learning (RL) methods.