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Efficient plasmon-hot electron conversion in Ag-CsPbBr3 hybrid nanocrystals.

ABSTRACT: Hybrid metal/semiconductor nano-heterostructures with strong exciton-plasmon coupling have been proposed for applications in hot carrier optoelectronic devices. However, the performance of devices based on this concept has been limited by the poor efficiency of plasmon-hot electron conversion at the metal/semiconductor interface. Here, we report that the efficiency of interfacial hot excitation transfer can be substantially improved in hybrid metal semiconductor nano-heterostructures consisting of perovskite semiconductors. In Ag-CsPbBr3 nanocrystals, both the plasmon-induced hot electron and the resonant energy transfer processes can occur on a time scale of less than 100 fs with quantum efficiencies of 50?±?18% and 15?±?5%, respectively. The markedly high efficiency of hot electron transfer observed here can be ascribed to the increased metal/semiconductor coupling compared with those in conventional systems. These findings suggest that hybrid architectures of metal and perovskite semiconductors may be excellent candidates to achieve highly efficient plasmon-induced hot carrier devices.

SUBMITTER: Huang X

PROVIDER: S-EPMC6411736 | biostudies-literature | 2019 Mar

REPOSITORIES: biostudies-literature

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Efficient plasmon-hot electron conversion in Ag-CsPbBr<sub>3</sub> hybrid nanocrystals.

Huang Xinyu X Li Hongbo H Zhang Chunfeng C Tan Shijing S Chen Zhangzhang Z Chen Lan L Lu Zhenda Z Wang Xiaoyong X Xiao Min M

Nature communications 20190311 1

Hybrid metal/semiconductor nano-heterostructures with strong exciton-plasmon coupling have been proposed for applications in hot carrier optoelectronic devices. However, the performance of devices based on this concept has been limited by the poor efficiency of plasmon-hot electron conversion at the metal/semiconductor interface. Here, we report that the efficiency of interfacial hot excitation transfer can be substantially improved in hybrid metal semiconductor nano-heterostructures consisting ...[more]

PMID: 30858372

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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.

Dataset Information

Efficient plasmon-hot electron conversion in Ag-CsPbBr3 hybrid nanocrystals.

Publications

Efficient plasmon-hot electron conversion in Ag-CsPbBr<sub>3</sub> hybrid nanocrystals.

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