Random Forest Predictor for Diblock Copolymer Phase Behavior

• Published in: ACS macro letters 2021-11, Vol.10 (11), p.1339-1345
• Main Authors: Arora, Akash, Lin, Tzyy-Shyang, Rebello, Nathan J, Av-Ron, Sarah H. M, Mochigase, Hidenobu, Olsen, Bradley D
• Format: Article
• Language: English
• ISSN: 2161-1653; 2161-1653
• DOI: 10.1021/acsmacrolett.1c00521

Physics-based models are the primary approach for modeling the phase behavior of block copolymers. However, the successful use of self-consistent field theory (SCFT) for designing new materials relies on the correct chemistry- and temperature-dependent Flory–Huggins interaction parameter χ AB that quantifies the incompatibility between the two blocks A and B as well as accurate estimation of the ratio of Kuhn lengths (b A/b B) and block densities. This work uses machine learning to model the phase behavior of AB diblock copolymers by using the chemical identities of blocks directly, obviating the need for measurement of χAB and b A/b B. The random forest approach employed predicts the phase behavior with almost 90% accuracy after training on a data set of 4768 data points, almost twice the accuracy obtained using SCFT employing χAB from group contribution theory. The machine-learning model is notably sensitive toward the uncertainty in measuring molecular parameters; however, its accuracy still remains at least 60% even for highly uncertain experimental measurements. Accuracy is substantially reduced when extrapolating to chemistries outside the training set. This work demonstrates that a random forest phase predictor performs remarkably well in many scenarios, providing an opportunity to predict self-assembly without measurement of molecular parameters.