Co-assembly of Lead Halide Perovskite Nanocrystals and Dielectric Nanodiscs 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

^aDepartment of Chemistry and Applied Biosciences, Institute of Inorganic Chemistry, ETH Zürich, Zürich, Switzerland

^bLaboratory of Thin Films and Photovoltaics, Empa – Swiss Federal Laboratories for Materials Science and Technology, Ueberlandstrasse, 129, 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

Proceedings of International Conference on Emerging Light Emitting Materials (EMLEM22)

Materials for next generation LEDs and lasers:

Limasol, Cyprus, 2022 October 3rd - 5th

Organizers: Maksym Kovalenko, Maryna Bodnarchuk and Grigorios Itskos

Poster, Chenglian Zhu, 012
Publication date: 15th July 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 as sharp, monodisperse cubes with tunable edge length making them attractive candidates as building blocks for self-assembly. A new step toward unique positional and orientational order would be to combine nanocubes with 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 CsPbBr₃ 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 CsPbBr₃ 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 CsPbBr₃ NCs resulted in the orthorhombic SL resembling the CaC₂ structure. For this 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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