Strongly Confined CsPbBr3 Perovskite Quantum Dots as Quantum Emitters and Building Blocks for Highly Ordered Rhombic Superlattices

Simon Boehme^a^,^b, Maryna Bodnarchuk^a^,^b, Max Burian^c, Federica Bertolotti^d, Ihor Cherniukh^a^,^b, Caterina Bernasconi^a^,^b, Chenglian Zhu^a^,^b, Heinz Amenitsch^f, Denys Naumenko^f, Hordii Andrusiv^a^,^b, Nazar Semkiv^a^,^b, Rohit Abraham John^a^,^b, Alan Baldwin^g^,^h, Krzystof Galkowski^g^,^h, Norberto Masciocchi^d, Samuel Stranks^g^,^h, Gabriele Rainò^a^,^b, Antonietta Guagliardi^e, Maksym Kovalenko^a^,^b

^aInstitute of Inorganic Chemistry, Department of Chemistry and Applied Biosciences, ETH Zürich, 8093 Zürich, Switzerland

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

^cSwiss Light Source, Paul Scherrer Institute, 5232 Villigen, Switzerland

^dDepartment of Science and High Technology and To.Sca.Lab., University of Insubria, via Valleggio 11, 22100 Como, Italy, Via Valleggio, 11, Como, Italy

^eIstituto di Cristallografia and To.Sca.Lab, Consiglio Nazionale delle Ricerche, Via Valleggio, 11, Como, Italy

^fInstitute of Inorganic Chemistry, Graz University of Technology, 8010 Graz, Austria

^gCavendish Laboratory, University of Cambridge, JJ Thomson Avenue, Cambridge CB3 0HE, U.K.

^hDepartment of Chemical Engineering & Biotechnology University of Cambridge, Philippa Fawcett Drive, United Kingdom

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, Simon Boehme, presentation 005
DOI: https://doi.org/10.29363/nanoge.emlem.2022.005
Publication date: 15th July 2022

The success of the colloidal semiconductor quantum dot (QD) field is rooted in the precise synthetic control of QD size, shape, and composition, enabling electronically well-defined functional nanomaterials that foster fundamental science and drive diverse fields of applications. While the exploitation of the strong confinement regime has been driving commercial and scientific interest in more traditional (e.g. InP or CdSe) QDs, a thorough exploration of such a regime has still not been achieved for lead-halide perovskite QDs. Here, we overcome previous challenges of insufficient chemical stability and monodispersity of small perovskite QDs via a post-synthetic treatment employing didodecyldimethylamonium bromide ligands. The achieved high monodispersity in both size and shape enables us to prepare self-assembled QD superlattices of exceptional long-range order and uniform thickness, with an unusual rhombic packing, and with narrow-band cyan emission. Their enhanced chemical stability allows us to explore strongly confined perovskite QDs at the single-particle/single-photon level.

Acknowledgements:

This work was partially supported by the European Union’s Horizon 2020 program through a FET Open research and innovation action (grant agreement No. 899141, PoLLoC), by the Swiss National Science Foundation (grant number 200021_192308, project Q-Light), and by the Air Force Office of Scientific Research and the Office of Naval Research (award number FA8655-21-1-7013). The authors are grateful for the use of facilities at the Empa Electron Microscopy Center. The authors acknowledge the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation program (HYPERION, grant agreement number 756962). F.B. acknowledges support by Fondazione Cariplo (Project 2020-4382). S.D.S. acknowledges funding from the Royal Society and the Tata Group (UF150033). A.B. acknowledges a Robert Gardiner Scholarship and funding from Christ’s College, Cambridge.

We acknowledge Joël Affolter for help with implementing the changepoint analysis utilized for the QD blinking studies. Antonio Cervellino and the technical staff of the MS-X04SA beamline of the Swiss Light Source (Paul Scherrer Institute, CH) are acknowledged for WAXTS measurements.

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