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Access to a blossoming library of colloidal nanomaterials provides building blocks for complex assembled materials. The journey to bring these prospects to fruition stands to benefit from the application of advanced processing methods. Epitaxially connected nanocrystal (or quantum dot) superlattices present a captivating model system for mesocrystals with intriguing emergent properties. The conventional processing approach to creating these materials involves assembling and attaching the constituent nanocrystals at the interface between two immiscible fluids. Processing small liquid volumes of the colloidal nanocrystal solution involves several complexities arising from the concurrent spreading, evaporation, assembly, and attachment. The ability of inkjet printers to deliver small (typically picoliter) liquid volumes with precise positioning is attractive to advance fundamental insights into the processing science, and thereby potentially enable new routes to incorporate the epitaxially connected superlattices into technology platforms. In this study, we identified the processing window of opportunity, including nanocrystal ink formulation and printing approach to enable delivery of colloidal nanocrystals from an inkjet nozzle onto the surface of a sessile droplet of the immiscible subphase. We demonstrate how inkjet printing can be scaled-down to enable the fabrication of epitaxially connected superlattices on patterned sub-millimeter droplets. We anticipate that insights from this work will spur on future advances to enable more mechanistic insights into the assembly processes and new avenues to create high-fidelity superlattices.
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