Structural Diversity in Multicomponent Nanocrystal Superlattices Comprising Lead Halide Perovskite Nanocubes

Ihor Cherniukh^a^,^b, Taras V. Sekh^a^,^b, Gabriele Rainò^a^,^b, Thilo Stöferle^c, Max Burian^d, Olivia J. Ashton^e, Rohit Abraham John^a^,^b, Alex Travesset^f, Chenglian Zhu^a^,^b, Etsuki Kobiyama^c, Yevhen Shynkarenko^a^,^b, Denys Naumenko^g, Heinz Amenitsch^g, Rolf Erni^e, Rainer F. Mahrt^c, Maryna I. Bodnarchuk^a^,^b, Maksym V. 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

^dSwiss Light Source, Paul Scherrer Institute, 5232 Villigen PSI, Switzerland

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

^fDepartment of Physics and Astronomy and Ames Laboratory, Iowa State University, Ames, 50011 Iowa, United States

^gInstitute of Inorganic Chemistry, Graz University of Technology, Stremayrgasse, 9, Graz, Austria

Materials for Sustainable Development Conference (MATSUS)
Proceedings of nanoGe Spring Meeting 2022 (NSM22)

#PerNC22. Colloidal Metal Halide Perovskite Nanocrystals: From Synthesis to Applications

Online, Spain, 2022 March 7th - 11th

Organizers: Maksym Kovalenko, Maryna Bodnarchuk and Osman Bakr

Contributed talk, Ihor Cherniukh, presentation 165
DOI: https://doi.org/10.29363/nanoge.nsm.2022.165
Publication date: 7th February 2022

Self-assembly of colloidal nanocrystals into long-range ordered superlattices holds great promise in the multiscale engineering of solid-state materials with controlled and programmed functionalities which result not only from combination and enhancement of size-dependent properties of constituent building blocks but also from synergistic effects and novel interactions between neighboring nanocrystals. Thus far, the reports had mainly focused on single-component and binary systems of spherical NCs, yielding SLs isostructural with the known atomic lattices [1]. Far greater structural space is anticipated from combining nanocrystals of various shapes. Caesium lead halide perovskite nanocrystals, possessing unique optoelectronic properties (narrow-band tunable bright emission, high oscillator strength of bright triplet excitons, slow dephasing) and being synthetically available as uniform, monodisperse cubes, are promising building blocks for creating superlattice structures that exhibit collective optical properties.

We show that broad structural diversity enabling effective tuning of the relative position and orientation of sub-10 nm CsPbBr₃ nanocubes can be achieved by their co-assembly with spherical, truncated cuboid and disk-shaped building blocks into long-range ordered multicomponent superlattices. CsPbBr₃ nanocubes combined with spherical Fe₃O₄ or NaGdF₄ nanocrystals and truncated cuboid PbS nanocrystals form binary SLs of six structure types, namely, NaCl-, AlB₂-, CuAu- as well as uncommon to all-sphere assemblies novel AB₂-, quasi-ternary ABO₃- and ABO₆-types. In these structures, nanocubes preserve orientational coherence. Co-assembly of CsPbBr₃ nanocudes with larger disk-shaped LaF₃ NCs (1.6 nm in thickness) results in the formation of seven columnar and lamellar structures with A₂B, AB, AB₂, AB₄ and AB₆ stoichiometry, not observed before for systems comprising spheres and disks. We rationalize the effect of the cubic shape on assembly outcome using packing-density calculations. In the systems with comparable dimensions of nanocubes (8.6 nm) and nanodisks (6.5–12.5 nm), other, non-columnar structures are observed, such as ReO₃-type SL, featuring intimate intermixing and face-to-face alignment of disks and cubes.

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.; Rainò, G.; Stöferle, T.; Burian, M.; Travesset, A.; Naumenko, D.; Amenitsch, H.; Erni, R.; Mahrt, R. F.; Bodnarchuk, M. I.; Kovalenko, M. V. Perovskite-Type Superlattices from Lead Halide Perovskite Nanocubes. Nature 2021, 593, 535-542.

[3] 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.

Acknowledgements:

This work was supported by the Swiss National Science Foundation (grant number 200021_192308, project Q-Light) and, in part, by the European Union through Horizon 2020 Research and Innovation Programme (ERC CoG Grant, grant agreement number 819740, project SCALE-HALO) and by the Air Force Office of Scientific Research under award number FA8655-21-1-7013. We acknowledge the funding received from EU-H2020 under grant agreement number 654360 supporting the Transnational Access Activity within the framework NFFA-Europe to the TUG’s ELETTRA SAXS beamline of CERIC-ERIC. We acknowledge the funding received from NSF, DMR-CMMT 1606336 (USA).

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