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Low-Temperature Molten Salts Synthesis: CsPbBr₃ Nanocrystals with High Photoluminescence Emission Buried in Mesoporous SiO₂.

ABSTRACT: Using mesoporous SiO₂ to encapsulate CsPbBr₃ nanocrystals is one of the best strategies to exploit such materials in devices. However, the CsPbBr₃/SiO₂ composites produced so far do not exhibit strong photoluminescence emission and, simultaneously, high stability against heat and water. We demonstrate a molten-salts-based approach delivering CsPbBr₃/mesoporous-SiO₂ composites with high PLQY (89 ± 10%) and high stability against heat, water, and aqua regia. The molten salts enable the formation of perovskite nanocrystals and other inorganic salts (KNO₃-NaNO₃-KBr) inside silica and the sealing of SiO₂ pores at temperatures as low as 350 °C, representing an important technological advancement (analogous sealing was observed only above 700 °C in previous reports). Our CsPbBr₃/mesoporous-SiO₂ composites are attractive for different applications: as a proof-of-concept, we prepared a white-light emitting diode exhibiting a correlated color temperature of 7692K. Our composites are also stable after immersion in saline water at high temperatures (a typical underground environment of oil wells), therefore holding promise as oil tracers.

SUBMITTER: An MN

PROVIDER: S-EPMC8025713 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:Ligand-capped nanocrystals (NCs) of lead halide perovskites, foremost fully inorganic CsPbX3 NCs, are the latest generation of colloidal semiconductor quantum dots. They offer a set of compelling characteristics-large absorption cross section, as well as narrow, fast, and efficient photoluminescence with long exciton coherence times-rendering them attractive for applications in light-emitting devices and quantum optics. Monodisperse and shape-uniform, broadly size-tunable, scalable, and robust NC samples are paramount for unveiling their basic photophysics, as well as for putting them into use. Thus far, no synthesis method fulfilling all these requirements has been reported. For instance, long-chain zwitterionic ligands impart the most durable surface coating, but at the expense of reduced size uniformity of the as-synthesized colloid. In this work, we demonstrate that size-selective precipitation of CsPbBr3 NCs coated with a long-chain sulfobetaine ligand, namely, 3-(N,N-dimethyloctadecylammonio)-propanesulfonate, yields monodisperse and sizable fractions (>100 mg inorganic mass) with the mean NC size adjustable in the range between 3.5 and 16 nm and emission peak wavelength between 479 and 518 nm. We find that all NCs exhibit an oblate cuboidal shape with the aspect ratio of 1.2 × 1.2 × 1. We present a theoretical model (effective mass/k·p) that accounts for the anisotropic NC shape and describes the size dependence of the first and second excitonic transition in absorption spectra and explains room-temperature exciton lifetimes. We also show that uniform zwitterion-capped NCs readily form long-range ordered superlattices upon solvent evaporation. In comparison to more conventional ligand systems (oleic acid and oleylamine), supercrystals of zwitterion-capped NCs exhibit larger domain sizes and lower mosaicity. Both kinds of supercrystals exhibit superfluorescence at cryogenic temperatures-accelerated collective emission arising from the coherent coupling of the emitting dipoles.

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Low-Temperature Molten Salts Synthesis: CsPbBr₃ Nanocrystals with High Photoluminescence Emission Buried in Mesoporous SiO₂.

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Low-Temperature Molten Salts Synthesis: CsPbBr3 Nanocrystals with High Photoluminescence Emission Buried in Mesoporous SiO2.

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OmicsDI is part of the ELIXIR infrastructure

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Low-Temperature Molten Salts Synthesis: CsPbBr₃ Nanocrystals with High Photoluminescence Emission Buried in Mesoporous SiO₂.