All-Perovskite Multicomponent Nanocrystal Superlattices

Sekh, Taras V.; Cherniukh, Ihor; Kobiyama, Etsuki; Sheehan, Thomas J.; Manoli, Andreas; Zhu, Chenglian; Athanasiou, Modestos; Sergides, Marios; Ortikova, Oleksandra; Rossell, Marta D.; Bertolotti, Federica; Guagliardi, Antonietta; Masciocchi, Norberto; Erni, Rolf; Othonos, Andreas; Itskos, Grigorios; Tisdale, William A.; Stöferle, Thilo; Rainò, Gabriele; Bodnarchuk, Maryna I.; Kovalenko, Maksym V.

doi:10.1021/acsnano.3c13062

Title: All-Perovskite Multicomponent Nanocrystal Superlattices

Journal Article · 05 March 2024 · ACS Nano

DOI: https://doi.org/10.1021/acsnano.3c13062 · OSTI ID:2471946

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Eidgenoessische Technische Hochschule (ETH), Zurich (Switzerland); Swiss Federal Laboratories for Materials Science and Technology (Empa), Dübendorf (Switzerland); OSTI
Eidgenoessische Technische Hochschule (ETH), Zurich (Switzerland); Swiss Federal Laboratories for Materials Science and Technology (Empa), Dübendorf (Switzerland)
IBM Research Europe−Zürich (Switzerland)
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
University of Cyprus, Nicosia (Cyprus)
Swiss Federal Laboratories for Materials Science and Technology (Empa), Dübendorf (Switzerland)
University of Insubria, Como (Italy)
Consiglio Nazionale delle Ricerche (CNR), Como (Italy)

Nanocrystal superlattices (NC SLs) have long been sought as promising metamaterials, with nanoscale-engineered properties arising from collective and synergistic effects among the constituent building blocks. Lead halide perovskite (LHP) NCs come across as outstanding candidates for SL design, as they demonstrate collective light emission, known as superfluorescence, in single- and multicomponent SLs. Thus far, LHP NCs have only been assembled in single-component SLs or coassembled with dielectric NC building blocks acting solely as spacers between luminescent NCs. Here, we report the formation of multicomponent LHP NC-only SLs, i.e., using only CsPbBr₃ NCs of different sizes as building blocks. The structural diversity of the obtained SLs encompasses the ABO₆, ABO₃, and NaCl structure types, all of which contain orientationally and positionally locked NCs. For the selected model system, the ABO₆-type SL, we observed efficient NC coupling and Förster-like energy transfer from strongly confined 5.3 nm CsPbBr₃ NCs to weakly confined 17.6 nm CsPbBr₃ NCs, along with characteristic superfluorescence features at cryogenic temperatures. Spatiotemporal exciton dynamics measurements reveal that binary SLs exhibit enhanced exciton diffusivity compared to single-component NC assemblies across the entire temperature range (from 5 to 298 K). The observed coherent and incoherent NC coupling and controllable excitonic transport within the solid NC SLs hold promise for applications in quantum optoelectronic devices.

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Research Organization:: Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)

Sponsoring Organization:: Swiss National Science Foundation (SNSF); US Air Force Office of Scientific Research (AFOSR); US Department of the Navy, Office of Naval Research (ONR); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0019345

OSTI ID:: 2471946

Journal Information:: ACS Nano, Journal Name: ACS Nano Journal Issue: 11 Vol. 18; ISSN 1936-0851

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
energy transfer
exciton diffusion
lead halide perovskites
nanocrystal coupling
nanocrystals
superfluorescence
superlattices

Title: All-Perovskite Multicomponent Nanocrystal Superlattices

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