Shape-Directed Co-Assembly of Lead Halide Perovskite Nanocubes into Superfluorescent Multicomponent Nanocrystal Superlattices

Ihor Cherniukh^a^,^b, Gabriele Rainò^a^,^b, Taras Sekh^a^,^b, Thilo Stöferle^c, Max Burian^d, Alex Travesset^e, Modestos Athanasiou^f, Andreas Manoli^f, Denys Naumenko^g, Heinz Amenitsch^g, Grigorios Itskos^f, Rolf Erni^h, 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, CH-8093 Zürich, 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

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

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

^fExperimental Condensed Matter Physics Laboratory, Department of Physics, University of Cyprus, 1678 Nicosia, Cyprus

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

^hElectron 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)

#NCFun23 - Fundamental Processes in Nanocrystals and 2D Materials

VALÈNCIA, Spain, 2023 March 6th - 10th

Organizers: Valerio Pinchetti and Shalini Singh

Oral, Ihor Cherniukh, presentation 258
DOI: https://doi.org/10.29363/nanoge.matsus.2023.258
Publication date: 22nd December 2022

Cesium lead halide perovskite nanocrystals, owing to their outstanding optoelectronic properties (high oscillator strength of bright triplet excitons, slow dephasing, minimal inhomogeneous broadening of emission lines), are promising building blocks for creating superlattice structures that exhibit collective phenomena in their optical spectra. Thus far, only single-component superlattices with the simple cubic packing have been devised from these nanocrystals, which have been shown to exhibit superfluorescence – a collective emission resulting in a burst of photons with ultrafast radiative decay (ca. 20 ps) that could be tailored for use in ultrabright (quantum) light sources [1]. However, far broader structural engineerability of superlattices, required for programmable tuning of the collective emission and for building a theoretical framework can be envisioned from the recent advancements in colloidal science. We show that the co-assembly of cubic and spherical steric-stabilized nanocrystals is experimentally possible and that the cubic shape of perovskite nanocrystals leads to a vastly different outcome compared to all-spherical systems. Five superlattice structures have been obtained: novel AB₂, ABO₃, ABO₆, besides expected NaCl or common to all-sphere assemblies AlB₂ superlattices [2, 3]. In binary ABO₃ and ABO₆ superlattices, larger spherical nanocrystals occupy the A sites and smaller cubic CsPbBr₃ nanocrystals reside on the B and O sites. Targeted substitution of B-site nanocubes by truncated cuboid PbS nanocrystals leads to the exclusive formation of ternary perovskite-type ABO₃ superlattice. Truncated cuboid PbS NCs can occupy A-sites in binary ABO₃, NaCl, and AlB₂ SLs with smaller CsPbBr₃ nanocubes. All synthesized superlattices exhibit a high degree of orientational ordering of the CsPbBr₃ nanocubes. We also demonstrate the effect of superlattice structure on the collective optical properties. In addition, we explore the on-liquid assembly method that allows for obtaining free-floating SL films comprising perovskite nanocrystals.

References:

[1] Rainò, G.; Becker, M.A.; Bodnarchuk, M.I.; Mahrt, R.F.; Kovalenko, M.V.; Stöferle, T. Superfluorescence from lead halide perovskite quantum dot superlattices. Nature 2018, 563, 671–675.

[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; Sekh, T. V.; Rainò, 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.; Stöferle, 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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