Megalibraries: Supercharged acceleration of materials discovery

Megalibraries are centimeter-scale chips containing millions to billions of individual materials each with an individually addressable position, composition, and size. Megalibraries will accelerate both the synthesis and characterization steps required for new material discoveries. Here, we review the key nanolithography developments that enable megalibrary synthesis and highlight the superior level of synthetic control within individual particles made possible by miniaturizing reactors to the nanoscale and performing chemistry confined to attoliter volumes. Massive parallelization of tip-defined materials synthesis offers control over thousands to millions of unique nanomaterials simultaneously, and then properties of interest can be rapidly screened. Unexplored materials can be readily surveyed and discovered using megalibraries, generating unprecedentedly large amounts of data that can be used to train machine learning algorithms. This approach is poised to revolutionize materials discovery that can be further amplified with highly autonomous design strategies. Graphical abstract