Machine Learning Framework for Characterizing Processing-Structure Relationship in Block Copolymer Thin Films

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 morphology type, 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 developed to predict morphological features based on processing parameters such as solvent ratio, additive type, and additive ratio. GISAXS-based properties were predicted with strong performances ($R^2$ > 0.75), while AFM-based property predictions were less accurate ($R^2$ < 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.

Adaptive AI decision interface for autonomous electronic material discovery

AI-powered autonomous experimentation (AI/AE) can accelerate materials discovery but its effectiveness for electronic materials is hindered by data scarcity from lengthy and complex design-fabricate-test-analyze cycles. Unlike experienced human scientists, even advanced AI algorithms in AI/AE lack the adaptability to make informative real-time decisions with limited datasets. Here, we address this challenge by developing and implementing an AI decision interface on our AI/AE system. The central element of the interface is an AI advisor that performs real-time progress monitoring, data analysis, and interactive human-AI collaboration for actively adapting to experiments in different stages and types. We applied this platform to an emerging type of electronic materials-mixed ion-electron conducting polymers (MIECPs) -- to engineer and study the relationships between multiscale morphology and properties. Using organic electrochemical transistors (OECT) as the testing-bed device for evaluating the mixed-conducting figure-of-merit -- the product of charge-carrier mobility and the volumetric capacitance ({\mu}C*), our adaptive AI/AE platform achieved a 150% increase in {\mu}C* compared to the commonly used spin-coating method, reaching 1,275 F cm-1 V-1 s-1 in just 64 autonomous experimental trials. A study of 10 statistically selected samples identifies two key structural factors for achieving higher volumetric capacitance: larger crystalline lamellar spacing and higher specific surface area, while also uncovering a new polymer polymorph in this material.

Machine Learning for Analyzing Atomic Force Microscopy (AFM) Images Generated from Polymer Blends

In this paper we present a new machine learning workflow with unsupervised learning techniques to identify domains within atomic force microscopy images obtained from polymer films. The goal of the workflow is to identify the spatial location of the two types of polymer domains with little to no manual intervention and calculate the domain size distributions which in turn can help qualify the phase separated state of the material as macrophase or microphase ordered or disordered domains. We briefly review existing approaches used in other fields, computer vision and signal processing that can be applicable for the above tasks that happen frequently in the field of polymer science and engineering. We then test these approaches from computer vision and signal processing on the AFM image dataset to identify the strengths and limitations of each of these approaches for our first task. For our first domain segmentation task, we found that the workflow using discrete Fourier transform or discrete cosine transform with variance statistics as the feature works the best. The popular ResNet50 deep learning approach from computer vision field exhibited relatively poorer performance in the domain segmentation task for our AFM images as compared to the DFT and DCT based workflows. For the second task, for each of 144 input AFM images, we then used an existing porespy python package to calculate the domain size distribution from the output of that image from DFT based workflow. The information and open source codes we share in this paper can serve as a guide for researchers in the polymer and soft materials fields who need ML modeling and workflows for automated analyses of AFM images from polymer samples that may have crystalline or amorphous domains, sharp or rough interfaces between domains, or micro or macrophase separated domains.