Escaping the Hydrolysis Trap: An Agentic Workflow for Inverse Design of Durable Photocatalytic Covalent Organic Frameworks

Covalent organic frameworks (COFs) are promising photocatalysts for solar hydrogen production, yet the most electronically favorable linkages, imines, hydrolyze rapidly in water, creating a stability--activity trade-off that limits practical deployment. Navigating the combinatorial design space of nodes, linkers, linkages, and functional groups to identify candidates that are simultaneously active and durable remains a formidable challenge. Here we introduce Ara, a large-language-model (LLM) agent that leverages pretrained chemical knowledge, donor--acceptor theory, conjugation effects, and linkage stability hierarchies, to guide the search for photocatalytic COFs satisfying joint band-gap, band-edge, and hydrolytic-stability criteria. Evaluated against random search and Bayesian optimization (BO) over a space consisting of candidates with various nodes, linkers, linkages, and r-groups, screened with a GFN1-xTB fragment pipeline, Ara achieves a 52.7\% hit rate (11.5$\times$ random, p = 0.006), finds its first hit at iteration 12 versus 25 for random search, and significantly outperforms BO (p = 0.006). Inspection of the agent's reasoning traces reveals interpretable chemical logic: early convergence on vinylene and beta-ketoenamine linkages for stability, node selection informed by electron-withdrawing character, and systematic R-group optimization to center the band gap at 2.0 eV. Exhaustive evaluation of the full search space uncovers a complementary exploitation--exploration trade-off between the agent and BO, suggesting that hybrid strategies may combine the strengths of both approaches. These results demonstrate that LLM chemical priors can substantially accelerate multi-criteria materials discovery.

ChemNavigator: Agentic AI Discovery of Design Rules for Organic Photocatalysts

The discovery of high-performance organic photocatalysts for hydrogen evolution remains limited by the vastness of chemical space and the reliance on human intuition for molecular design. Here we present ChemNavigator, an agentic AI system that autonomously derives structure-property relationships through hypothesis-driven exploration of organic photocatalyst candidates. The system integrates large language model reasoning with density functional tight binding calculations in a multi-agent architecture that mirrors the scientific method: formulating hypotheses, designing experiments, executing calculations, and validating findings through rigorous statistical analysis. Through iterative discovery cycles encompassing 200 molecules, ChemNavigator autonomously identified six statistically significant design rules governing frontier orbital energies, including the effects of ether linkages, carbonyl groups, extended conjugation, cyano groups, halogen substituents, and amine groups. Importantly, these rules correspond to established principles of organic electronic structure (resonance donation, inductive withdrawal, $π$-delocalization), demonstrating that the system can independently derive chemical knowledge without explicit programming. Notably, autonomous agentic reasoning extracted these six validated rules from a molecular library where previous ML approaches identified only carbonyl effects. Furthermore, the quantified effect sizes provide a prioritized ranking for synthetic chemists, while feature interaction analysis revealed diminishing returns when combining strategies, challenging additive assumptions in molecular design. This work demonstrates that agentic AI systems can autonomously derive interpretable, chemically grounded design principles, establishing a framework for AI-assisted materials discovery that complements rather than replaces chemical intuition.

Artificial Intelligence in Materials Science and Engineering: Current Landscape, Key Challenges, and Future Trajectorie

Artificial Intelligence is rapidly transforming materials science and engineering, offering powerful tools to navigate complexity, accelerate discovery, and optimize material design in ways previously unattainable. Driven by the accelerating pace of algorithmic advancements and increasing data availability, AI is becoming an essential competency for materials researchers. This review provides a comprehensive and structured overview of the current landscape, synthesizing recent advancements and methodologies for materials scientists seeking to effectively leverage these data-driven techniques. We survey the spectrum of machine learning approaches, from traditional algorithms to advanced deep learning architectures, including CNNs, GNNs, and Transformers, alongside emerging generative AI and probabilistic models such as Gaussian Processes for uncertainty quantification. The review also examines the pivotal role of data in this field, emphasizing how effective representation and featurization strategies, spanning compositional, structural, image-based, and language-inspired approaches, combined with appropriate preprocessing, fundamentally underpin the performance of machine learning models in materials research. Persistent challenges related to data quality, quantity, and standardization, which critically impact model development and application in materials science and engineering, are also addressed.

Teaching Artificial Intelligence to Perform Rapid, Resolution-Invariant Grain Growth Modeling via Fourier Neural Operator

Microstructural evolution, particularly grain growth, plays a critical role in shaping the physical, optical, and electronic properties of materials. Traditional phase-field modeling accurately simulates these phenomena but is computationally intensive, especially for large systems and fine spatial resolutions. While machine learning approaches have been employed to accelerate simulations, they often struggle with resolution dependence and generalization across different grain scales. This study introduces a novel approach utilizing Fourier Neural Operator (FNO) to achieve resolution-invariant modeling of microstructure evolution in multi-grain systems. FNO operates in the Fourier space and can inherently handle varying resolutions by learning mappings between function spaces. By integrating FNO with the phase field method, we developed a surrogate model that significantly reduces computational costs while maintaining high accuracy across different spatial scales. We generated a comprehensive dataset from phase-field simulations using the Fan Chen model, capturing grain evolution over time. Data preparation involved creating input-output pairs with a time shift, allowing the model to predict future microstructures based on current and past states. The FNO-based neural network was trained using sequences of microstructures and demonstrated remarkable accuracy in predicting long-term evolution, even for unseen configurations and higher-resolution grids not encountered during training.