High-Throughput Screening and Prediction of High Modulus of Resilience Polymers Using Explainable Machine Learning

TL Yue and JL He and L Tao and Y Li, JOURNAL OF CHEMICAL THEORY AND COMPUTATION, 19, 4641-4653 (2023).

DOI: 10.1021/acs.jctc.3c00131

The ability to store and release elastic strain energy, as well as mechanical strength, are crucial factors in both natural and man-made mechanical systems. The modulus of resilience (R) indicates a material's capacity to absorb and release elastic strain energy, with the yield strength (sy) and Young's modulus (E) as R = sy2/(2E) for linear elastic solids. To improve the R in linear elastic solids, a high sy and low E combination in materials is sought after. However, achieving this combination is a significant challenge as both properties typically increase together. To address this challenge, we propose a computational method to quickly identify polymers with a high modulus of resilience using machine learning (ML) and validate the predictions through high- fidelity molecular dynamics (MD) simulations. Our approach commences by training single-task ML models, multitask ML models, and Evidential Deep Learning models to forecast the mechanical properties of polymers based on experimentally reported values. Utilizing explainable ML models, we were able to determine the critical substructures that significantly impact the mechanical properties of polymers, such as E and sy. This information can be utilized to create and develop new polymers with improved mechanical characteristics. Our single-task and multitask ML models can predict the properties of 12 854 real polymers and 8 million hypothetical polyimides and uncover 10 new real polymers and 10 hypothetical polyimides with exceptional modulus of resilience. The improved modulus of resilience of these novel polymers was validated through MD simulations. Our method efficiently speeds up the discovery of high-performing polymers using ML predictions and MD validation and can be applied to other polymer material discovery challenges, such as polymer membranes, dielectric polymers, and more.

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