High-Throughput Experimentation for The Exploration of High Entropy Materials: From Alloys to Oxides and Nitrides

Discovery of new materials is a key challenge in materials science. New materials for sustainable production/storage/conversion of energy carriers are necessary to improve existing and to enable future energy systems. Compositionally complex materials, frequently called high entropy materials, offer a vast multidimensional search space, which provides opportunities for discovering new materials. Next to alloys compounds such as oxides and nitrides are of interest. However, efficient methods for the exploration and exploitation of this multidimensional search space are necessary, especially as oxides and nitrides need more sophisticated synthesis methods such as reactive sputter deposition. Here, the integration of high-throughput thin-film combinatorial materials science methods with simulation and materials informatics (1) is presented as an effective means to produce large datasets on new materials, which enables mastering of this immense search space. The approach combines theoretical predictions from high-throughput computations with production of large, consistent and complete experimental datasets, which are used for materials informatics. Thin-film materials libraries are fabricated by (reactive) combinatorial sputter deposition and optional post-deposition treatments, followed by high-throughput characterization, and finally the organization of the acquired multi-dimensional data in adequate databases as well their effective computational analysis and visualization, e.g., of polyelemental systems in the form of composition-processing-structure-function diagrams, interlinking compositional data with structural and functional properties. The talk will discuss examples of high-throughput exploration of compositionally complex metallic solid solutions as well as oxide and nitride thin-film libraries for electrocatalysis and solar water splitting (2-7). In the case of compositionally complex perovskites, we recently discovered a new platform for materials discovery (8). Furthermore, a new approach (9) to accelerate atomic-scale measurements for complex materials and their oxidation (10) is presented.<br/><br/>(1) A. Ludwig (2019), npj computational materials 5, 70<br/>(2) T. Löffler et al. (2018), Adv. Energy Mater. 8, 1802269<br/>(3) T. A. A. Batchelor et al. (2021) Angewandte Chemie 60, 6932–6937<br/>(4) V. Strotkötter et al. (2022), Chemistry of Materials, 34, 10291-10303<br/>(5) E. Suhr et al. (2023), Advanced Engineering Materials 300550<br/>(6) S. Kumari et al. (2020), Zeitschrift für Physikalische Chemie 234, 867-885<br/>(7) M. Nowak, et al. (2020), Zeitschrift für Physikalische Chemie 234, 835-845<br/>(8) T. H. Piotrowiak et al., (2023), Advanced Engineering Materials 25, 2300437<br/>(9) Y. J. Li et al.. (2018), Materials Horizons 5, 86 - 92<br/>(10) Y. Li et al.. (2018), J. Alloys and Compounds 766, 1080 -1085