Co-assembly of Shape Anisotropic Lead Halide Perovskite and Dielectric Nanocrystals into Multicomponent Functional Superlattices

Taras Sekh^a^,^b, Ihor Cherniukh^a^,^b, Gabriele Rainò^a^,^b, Chenglian Zhu^a^,^b, Yevhen Shynkarenko^a^,^b, Rohit Abraham John^a^,^b, Olivia Ashton^d, Etsuki Kobiyama^c, Rainer Mahrt^c, Thilo Stöferle^c, Rolf Erni^d, Maryna Bodnarchuk^a^,^b, Maksym Kovalenko^a^,^b

^aETH Zürich, Department of Chemistry and Applied Biosciences, CH-8093, Zurich, Switzerland

^bLaboratory for Thin Films and Photovoltaics, Empa – Swiss Federal Laboratories for Materials Science and Technology, CH-8600 Dübendorf, Switzerland

^cIBM Research Europe — Zurich, Säumerstrasse, 4, Rüschlikon, Switzerland

^dElectron Microscopy Center, Empa – Swiss Federal Laboratories for Materials Science and Technology, Ueberlandstrasse, 129, Dübendorf, Switzerland

Materials for Sustainable Development Conference (MATSUS)
Proceedings of MATSUS23 & Sustainable Technology Forum València (STECH23) (MATSUS23)

#ChemNano23 - Chemistry of Nanomaterials

VALÈNCIA, Spain, 2023 March 6th - 10th

Organizers: Loredana Protesescu and Maksym Yarema

Oral, Taras Sekh, presentation 252
DOI: https://doi.org/10.29363/nanoge.matsus.2023.252
Publication date: 22nd December 2022

Self-assembly of colloidal nanocrystals into long-range-ordered structures through a bottom-up approach is highly promising for creating metamaterials with programmable functionalities arising from various synergistic effects and emergent interactions between neighboring NCs. Both single-component and binary superlattices reported so far were mainly composed of spherical NCs limiting the variety of obtained structures to the ones isostructural with the known atomic lattices [1]. A far greater structural diversity is accessible via assembling NCs of different shapes, e.g. nanoplates, nanorods, nanocubes, or nanodiscs. Notably, lead halide perovskite nanocrystals are characterized by remarkable optical properties together with being synthetically available in the monodisperse form making them attractive candidates as building blocks for self-assembly. A new step toward unique positional and orientational order would be to combine perovskite NCs with dielectric NCs of anisotropic shape. To this end, we have chosen LaF₃ and NaGdF₄ NCs as a second component for SLs due to their synthetic accessibility and well-defined, ensemble-uniform morphology.

Co-assembly of cesium lead halide nanocubes with disc-shaped LaF₃ NCs (9.2-28.4 nm in diameter) leads to the formation of six columnar structures with AB, AB₂, AB₄, and AB₆ stoichiometry as well as to noncolumnar lamellar and ReO₃-type SLs by employing larger perovskite NCs [2]. The latter two SLs proved to exhibit characteristic features of the collective ultrafast emission – superfluorescence. Intending to broaden the variety of building blocks for NC SLs, we utilized organic-inorganic perovskite NCs, namely FAPbBr₃ NCs, for the formation of binary SLs with spherical NaGdF₄ NCs (b-ABO₃-, AlB₂-, AB₂-, NaCl-type structures) and LaF₃ nanodiscs (columnar AB-type and lamellar SLs). Combining larger and thicker NaGdF₄ nanodiscs (18.5 nm in thickness) with cesium lead halide NCs resulted in the CaC₂-like and AB₃-type SLs. For CaC₂- and ABO₃-type structures, we expanded the scope of the available dimensionalities of SLs by employing microemulsion-templated self-assembly which allowed for the formation of three-dimensional binary supraparticles [3].

References:

[1] Boles, M.; Engel, M.; Talapin, D. Self-Assembly of Colloidal Nanocrystals: From Intricate Structures to Functional Materials. Chem. Rev. 2016, 116, 18, 11220–11289.

[2] Cherniukh, I.; Raino, G.; Sekh, T. V.; Zhu, C.; Shynkarenko, Y.; John, R. A.; Kobiyama, E.; Mahrt, R. F.; Stoferle, T.; Erni, R.; Kovalenko, M. V.; Bodnarchuk, M. I. Shape-Directed Co-Assembly of Lead Halide Perovskite Nanocubes with Dielectric Nanodisks into Binary Nanocrystal Superlattices. ACS Nano 2021, 15, 10, 16488–16500.

[3] Cherniukh, I.; Sekh, T. V.; Raino, G.; Ashton, O. J.; Burian, M.; Travesset, A.; Athanasiou, M.; Manoli, A.; John, R. A.; Svyrydenko, M.; Morad, V.; Shynkarenko, Y.; Montanarella, F.; Naumenko, D.; Amenitsch, H.; Itskos, G.; Mahrt, R. F.; Stoferle, T.; Erni, R.; Kovalenko, M. V.; Bodnarchuk, M. I. Structural Diversity in Multicomponent Nanocrystal Superlattices Comprising Lead Halide Perovskite Nanocubes. ACS Nano 2022, 16, 5, 7210–7232.

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