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Title: Machine Learning Framework for Characterizing Processing–Structure Relationship in Block Copolymer Thin Films

Journal Article · · Macromolecules

The morphology of block copolymers (BCPs) critically influences material properties and applications. This work introduces a machine learning (ML)-enabled, high-throughput framework for analyzing grazing incidence small-angle X-ray scattering (GISAXS) data and atomic force microscopy (AFM) images to characterize BCP thin film morphology. A convolutional neural network was trained to classify AFM images by surface features, achieving 97% testing accuracy. Classified images were then analyzed to extract 2D grain size measurements from the samples in a high-throughput manner. ML models were trained to predict domain orientation based on processing parameters such as solvent ratio, additive type, and additive ratio. GISAXS-based properties were predicted with strong performances (R2 > 0.75), while AFM-based property predictions were less accurate (R2 < 0.60), likely due to the localized nature of AFM measurements compared to the bulk information captured by GISAXS. Beyond model performance, interpretability was addressed using SHapley Additive exPlanations (SHAP). SHAP analysis revealed that the additive ratio had the largest impact on morphological predictions, where additive provides the BCP chains with increased volume to rearrange into thermodynamically favorable morphologies. This interpretability helps validate model predictions and offers insight into parameter importance. Altogether, the presented framework combining high-throughput characterization and interpretable ML offers an approach to exploring and optimizing BCP thin film morphology across a broad processing landscape.

Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); US Department of Energy (USDOE), Washington, DC (United States). Office of Science, Basic Energy Sciences (BES)
Sponsoring Organization:
National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)
Grant/Contract Number:
AC02-05CH11231; SC0012704; SC0024432
OSTI ID:
3015413
Report Number(s):
BNL--229366-2026-JAAM
Journal Information:
Macromolecules, Journal Name: Macromolecules Journal Issue: 2 Vol. 59; ISSN 1520-5835; ISSN 0024-9297
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English

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