Superfluorescent Multicomponent Nanocrystal Superlattices from Lead Halide Perovskite Nanocubes

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, Rohit John^a^,^b, Yevhen Shynkarenko^a^,^b, Denys Naumenko^g, Heinz Amenitsch^g, Grigorios Itskos^f, Rolf Erni^h, Rainer Mahrt^c, 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

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

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

Oral, Ihor Cherniukh, presentation 001
DOI: https://doi.org/10.29363/nanoge.emlem.2022.001
Publication date: 15th July 2022

Cesium lead halide perovskite nanocrystals, owing to high oscillator strength of bright triplet excitons, long coherence times and 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 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.

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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