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Resonantly enhanced multiple exciton generation through below-band-gap multi-photon absorption in perovskite nanocrystals

Author

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  • Aurora Manzi

    (Ludwig-Maximilians-Universität
    Nanosystems Initiative Munich (NIM))

  • Yu Tong

    (Ludwig-Maximilians-Universität
    Nanosystems Initiative Munich (NIM))

  • Julius Feucht

    (Ludwig-Maximilians-Universität
    Nanosystems Initiative Munich (NIM))

  • En-Ping Yao

    (Ludwig-Maximilians-Universität
    Nanosystems Initiative Munich (NIM))

  • Lakshminarayana Polavarapu

    (Ludwig-Maximilians-Universität
    Nanosystems Initiative Munich (NIM))

  • Alexander S. Urban

    (Ludwig-Maximilians-Universität
    Nanosystems Initiative Munich (NIM))

  • Jochen Feldmann

    (Ludwig-Maximilians-Universität
    Nanosystems Initiative Munich (NIM))

Abstract

Multi-photon absorption and multiple exciton generation represent two separate strategies for enhancing the conversion efficiency of light into usable electric power. Targeting below-band-gap and above-band-gap energies, respectively, to date these processes have only been demonstrated independently. Here we report the combined interaction of both nonlinear processes in CsPbBr3 perovskite nanocrystals. We demonstrate nonlinear absorption over a wide range of below-band-gap excitation energies (0.5–0.8 Eg). Interestingly, we discover high-order absorption processes, deviating from the typical two-photon absorption, at specific energetic positions. These energies are associated with a strong enhancement of the photoluminescence intensity by up to 105. The analysis of the corresponding energy levels reveals that the observed phenomena can be ascribed to the resonant creation of multiple excitons via the absorption of multiple below-band-gap photons. This effect may open new pathways for the efficient conversion of optical energy, potentially also in other semiconducting materials.

Suggested Citation

  • Aurora Manzi & Yu Tong & Julius Feucht & En-Ping Yao & Lakshminarayana Polavarapu & Alexander S. Urban & Jochen Feldmann, 2018. "Resonantly enhanced multiple exciton generation through below-band-gap multi-photon absorption in perovskite nanocrystals," Nature Communications, Nature, vol. 9(1), pages 1-6, December.
    • Handle: RePEc:nat:natcom:v:9:y:2018:i:1:d:10.1038_s41467-018-03965-8
    DOI: 10.1038/s41467-018-03965-8
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    Cited by:

    1. Yue Wang & Senyun Ye & Jia Wei Melvin Lim & David Giovanni & Minjun Feng & Jianhui Fu & Harish N S Krishnamoorthy & Qiannan Zhang & Qiang Xu & Rui Cai & Tze Chien Sum, 2023. "Carrier multiplication in perovskite solar cells with internal quantum efficiency exceeding 100%," Nature Communications, Nature, vol. 14(1), pages 1-9, December.

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