Previous research on multimaterial aerosol jet printing has made steady progress in the development of functional materials and devices 14, 15, although aerosol-based printing of combinatorial gradient materials remains challenging. However, these methods still suffer from limited materials options and challenges in regard to the universal combination of different materials and the production of gradient material libraries, due to the lack of fast mixing mechanisms and the inability to rapidly vary mixing ratios.įor an ideal interdiffusion system, low fluid viscosity and minimal size of diffusion units are desired, which leads us to investigate the potential of using aerosols for in situ mixing and printing. Recently several printing approaches, including inkjet printing, electrochemical printing and electrohydrodynamic redox printing, have been proposed for the fabrication of material libraries 11, 12, 13. Additive manufacturing has emerged as a versatile method to fabricate materials of complex structure using micro- and nanoscale building blocks 8, 9, 10. Nevertheless, the intrinsic high-energy nature of laser or plasma excludes many materials (for example, colloidal particles, thermosensitive polymers) from use in the development of universal combinatorial material libraries. The sample-rich feature of these combinatorial material libraries facilitates elucidation of the composition–structure–property relationship and enables the rapid screening of materials over a vast range of compositions. Combinatorial material depositions (for example, cosputtering) have enabled rapid screening of new materials for electronics, magnetics, optics and energy-related applications 7. Materials hold pivotal roles in many scientific and technological innovations, and progress in developing new materials is key to the pursuit of solutions to grand societal challenges. The ability to combine the top-down design freedom of additive manufacturing with bottom-up control over local material compositions promises the development of compositionally complex materials inaccessible via conventional manufacturing approaches. We demonstrate a variety of high-throughput printing strategies and applications in combinatorial doping, functional grading and chemical reaction, enabling materials exploration of doped chalcogenides and compositionally graded materials with gradient properties. In situ mixing and printing in the aerosol phase allows instantaneous tuning of the mixing ratio of a broad range of materials on the fly, which is an important feature unobtainable in conventional multimaterials printing using feedstocks in liquid–liquid or solid–solid phases 4, 5, 6. Here we report a high-throughput combinatorial printing method capable of fabricating materials with compositional gradients at microscale spatial resolution. Whereas traditional combinatorial deposition methods can generate material libraries 2, 3, these suffer from limited material options and inability to leverage major breakthroughs in nanomaterial synthesis. The Edisonian trial-and-error process is time consuming and resource inefficient, particularly when contrasted with vast materials design spaces 1. However, materials discovery and optimization have been a frustratingly slow process. The development of new materials and their compositional and microstructural optimization are essential in regard to next-generation technologies such as clean energy and environmental sustainability.
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