Po-Yen Tung

A tremendous range of design tasks in materials, physics, and biology can be formulated as finding the optimum of an objective function depending on many parameters without knowing its closed-form expression or the derivative. Traditional derivative-free optimization techniques often rely on strong assumptions about objective functions, thereby failing at optimizing non-convex systems beyond 100 dimensions. Here, we present a tree search method for derivative-free optimization that enables accelerated optimal design of high-dimensional complex systems. Specifically, we introduce stochastic tree expansion, dynamic upper confidence bound, and short-range backpropagation mechanism to evade local optimum, iteratively approximating the global optimum using machine learning models. This development effectively confronts the dimensionally challenging problems, achieving convergence to global optima across various benchmark functions up to 2,000 dimensions, surpassing the existing methods by 10- to 20-fold. Our method demonstrates wide applicability to a wide range of real-world complex systems spanning materials, physics, and biology, considerably outperforming state-of-the-art algorithms. This enables efficient autonomous knowledge discovery and facilitates self-driving virtual laboratories. Although we focus on problems within the realm of natural science, the advancements in optimization techniques achieved herein are applicable to a broader spectrum of challenges across all quantitative disciplines.

Identification of unknown micro- and nano-sized mineral phases is commonly achieved by analyzing chemical maps generated from hyperspectral imaging data sets, particularly scanning electron microscope—energy dispersive X-ray spectroscopy (SEM-EDS). However, the accuracy and reliability of mineral identification are often limited by subjective human interpretation, non-ideal sample preparation, and the presence of mixed chemical signals generated within the electron-beam interaction volume. Machine learning has emerged as a powerful tool to overcome these problems. Here, we propose a machine-learning approach to identify unknown phases and unmix their overlapped chemical signals. This approach leverages the guidance of Gaussian mixture modeling clustering fitted on an informative latent space of pixel-wise elemental data points modeled using a neural network autoencoder, and unmixes the overlapped chemical signals of phases using non-negative matrix factorization. We evaluate the reliability and the accuracy of the new approach using two SEM-EDS data sets: a synthetic mixture sample and a real-world particulate matter sample. In the former, the proposed approach successfully identifies all major phases and extracts background-subtracted single-phase chemical signals. The unmixed chemical spectra show an average similarity of 83.0% with the ground truth spectra. In the second case, the approach demonstrates the ability to identify potentially magnetic Fe-bearing particles and their background-subtracted chemical signals. We demonstrate a flexible and adaptable approach that brings a significant improvement to mineralogical and chemical analysis in a fully automated manner. The proposed analysis process has been built into a user-friendly Python code with a graphical user interface for ease of use by general users.

High-entropy alloys are solid solutions of multiple principal elements that are capable of reaching composition and property regimes inaccessible for dilute materials. Discovering those with valuable properties, however, too often relies on serendipity, because thermodynamic alloy design rules alone often fail in high-dimensional composition spaces. We propose an active learning strategy to accelerate the design of high-entropy Invar alloys in a practically infinite compositional space based on very sparse data. Our approach works as a closed-loop, integrating machine learning with density-functional theory, thermodynamic calculations, and experiments. After processing and characterizing 17 new alloys out of millions of possible compositions, we identified two high-entropy Invar alloys with extremely low thermal expansion coefficients around 2 × 10−6 per degree kelvin at 300 kelvin. We believe this to be a suitable pathway for the fast and automated discovery of high-entropy alloys with optimal thermal, magnetic, and electrical properties.