Flexible Polymer-Assisted Mesoscale Self-Assembly of Colloidal CsPbBr3 Perovskite Nanocrystals into Higher Order Superstructures with Strong Inter-Nanocrystal Electronic Coupling
dc.contributor.author | Yang, Yang | |
dc.contributor.author | Lee, Jacob T. | |
dc.contributor.author | Liyanage, Thakshila | |
dc.contributor.author | Sardar, Rajesh | |
dc.contributor.department | Chemistry and Chemical Biology, School of Science | en_US |
dc.date.accessioned | 2019-01-30T18:18:07Z | |
dc.date.available | 2019-01-30T18:18:07Z | |
dc.date.issued | 2019 | |
dc.description.abstract | Surface-passivating ligands, although ubiquitous to colloidal nanocrystal (NC) syntheses, play a role in assembling NCs into higher order structures and hierarchical superstructures, which has not been demonstrated yet for colloidal CsPbX3 (X = Cl, Br, and I) NCs. In this work, we report that functional poly(ethylene glycols) (PEG6-Y, Y = −COOH and −NH2) represent unique surface-passivating ligands enabling the synthesis of near-uniform CsPbBr3 NCs with diameters of 3.0 nm. The synthesized NCs are assembled into individual pearl necklaces, bundled pearl necklaces, lamellar, and nanorice superstructures, in situ. It is believed a variety of forces, including van der Waals attractions between hydrophilic PEG tails in a nonpolar solvent and dipole–dipole attraction between NCs, drive mesoscale assembly to form superstructures. Furthermore, postsynthetic ligand treatment strengthens the argument for polymer-assisted mesoscale assembly as pearl necklace assemblies can be successfully converted into either lamellar or nanorice structures. We observe an ∼240 meV bathochromic shift in the lowest energy absorption peak of CsPbBr3 NCs when they are present in the lamellar and nanorice assemblies, representing strong inter-NC electronic coupling. Moreover, pearl necklace structures are spontaneously assembled into micrometer length scale twisted ribbon hierarchical superstructures during storage of colloidal CsPbBr3 NCs. The results show that the self-assembled superstructures of CsPbBr3 NCs are now feasible to prepare via template-free synthesis, as self-assembled structures emerge in the bulk solvent, a process that mimics biological systems except for the use of nonbiological surface ligands (PEG6-Y). Taken together, emergent optoelectronic properties and higher order superstructures of CsPbBr3 NCs should aid their potential use in solid-state devices and simplify scalable manufacturing. | en_US |
dc.eprint.version | Author's manuscript | en_US |
dc.identifier.citation | Yang, Y., Lee, J. T., Liyanage, T., & Sardar, R. (2019). Flexible Polymer-Assisted Mesoscale Self-Assembly of Colloidal CsPbBr3 Perovskite Nanocrystals into Higher Order Superstructures with Strong Inter-Nanocrystal Electronic Coupling. Journal of the American Chemical Society. https://doi.org/10.1021/jacs.8b10083 | en_US |
dc.identifier.uri | https://hdl.handle.net/1805/18269 | |
dc.language.iso | en | en_US |
dc.publisher | ACS | en_US |
dc.relation.isversionof | 10.1021/jacs.8b10083 | en_US |
dc.relation.journal | Journal of the American Chemical Society | en_US |
dc.rights | Publisher Policy | en_US |
dc.source | Author | en_US |
dc.subject | template-free synthesis | en_US |
dc.subject | scalable manufacturing | en_US |
dc.subject | higher order superstructures | en_US |
dc.title | Flexible Polymer-Assisted Mesoscale Self-Assembly of Colloidal CsPbBr3 Perovskite Nanocrystals into Higher Order Superstructures with Strong Inter-Nanocrystal Electronic Coupling | en_US |
dc.type | Article | en_US |