Fundamental Processes and Practical Considerations of Lead Chalcogenide Mesocrystals Formed via Self-Assembly and Directed Attachment of Nanocrystals at a Fluid Interface

Cimada daSilva, Jessica; Balazs, Daniel M.; Dunbar, Tyler A.; Hanrath, Tobias

doi:10.1021/acs.chemmater.1c02910

Title: Fundamental Processes and Practical Considerations of Lead Chalcogenide Mesocrystals Formed via Self-Assembly and Directed Attachment of Nanocrystals at a Fluid Interface

Journal Article · Thu Dec 16 00:00:00 EST 2021 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.1c02910· OSTI ID:1836502

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Cornell Univ., Ithaca, NY (United States)
Cornell Univ., Ithaca, NY (United States); IST Austria, Klosterneuburg (Austria)

Significant advances in the synthesis and processing of colloidal nanocrystals have given scientists and engineers access to a vast library of building blocks with precisely defined size, shape, and composition. These materials have inspired exciting prospects to enable bottom-up fabrication of programmable materials with properties by design. Successfully assembling and connecting the building blocks into superstructures in which constituent nanocrystals can purposefully interact requires robust understanding of and control over a complex interplay of dynamic physicochemical processes. Fluid interfaces provide an advantageous experimental workbench to both probe and control these processes. Despite the ostensible simplicity of fabricating nanocrystal assemblies at a fluid interface, sensitivity to processing conditions and limited reproducibility have underscored the complexity of this process. In situ studies have provided mechanistic insights into the competing dynamics of key subprocesses including solvent spreading and evaporation, superlattice formation, ligand detachment kinetics, and nanocrystal attachment. Understanding how these subprocesses influence the complex choreography of self-assembly, structure transformation, and oriented attachment processes presents a rich research challenge. In this context, we present a detailed methodology for self-assembly and attachment of lead chalcogenide nanocrystals at a liquid–gas interface as a model system for the fabrication of mono- and multilayer cubic connected superlattices. We discuss key experimental parameters such as the characteristics of the building blocks and processing conditions and detailed steps from colloidal nanocrystal injection to superlattice transfer. Furthermore, we hope that this Methods/Protocols paper will provide guidance for future advances in the exciting path toward bringing the prospect of nanocrystal-based programmable materials to fruition.

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Research Organization:: Cornell Univ., Ithaca, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0018026

OSTI ID:: 1836502

Journal Information:: Chemistry of Materials, Vol. 33, Issue 24; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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