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Manipulation of hot carrier cooling dynamics in two-dimensional Dion–Jacobson hybrid perovskites via Rashba band splitting

Author

Listed:
  • Jun Yin

    (Advanced Membranes and Porous Materials Center, Division of Physical Science and Engineering, King Abdullah University of Science and Technology
    KAUST Catalysis Center, Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology)

  • Rounak Naphade

    (KAUST Catalysis Center, Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology)

  • Partha Maity

    (Advanced Membranes and Porous Materials Center, Division of Physical Science and Engineering, King Abdullah University of Science and Technology
    KAUST Catalysis Center, Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology)

  • Luis Gutiérrez-Arzaluz

    (Advanced Membranes and Porous Materials Center, Division of Physical Science and Engineering, King Abdullah University of Science and Technology
    KAUST Catalysis Center, Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology)

  • Dhaifallah Almalawi

    (Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology
    Taif University)

  • Iman S. Roqan

    (Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology)

  • Jean-Luc Brédas

    (The University of Arizona)

  • Osman M. Bakr

    (KAUST Catalysis Center, Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology)

  • Omar F. Mohammed

    (Advanced Membranes and Porous Materials Center, Division of Physical Science and Engineering, King Abdullah University of Science and Technology
    KAUST Catalysis Center, Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology)

Abstract

Hot-carrier cooling processes of perovskite materials are typically described by a single parabolic band model that includes the effects of carrier-phonon scattering, hot phonon bottleneck, and Auger heating. However, little is known (if anything) about the cooling processes in which the spin-degenerate parabolic band splits into two spin-polarized bands, i.e., the Rashba band splitting effect. Here, we investigated the hot-carrier cooling processes for two slightly different compositions of two-dimensional Dion–Jacobson hybrid perovskites, namely, (3AMP)PbI4 and (4AMP)PbI4 (3AMP = 3-(aminomethyl)piperidinium; 4AMP = 4-(aminomethyl)piperidinium), using a combination of ultrafast transient absorption spectroscopy and first-principles calculations. In (4AMP)PbI4, upon Rashba band splitting, the spin-dependent scattering of hot electrons is responsible for accelerating hot-carrier cooling at longer delays. Importantly, the hot-carrier cooling of (4AMP)PbI4 can be extended by manipulating the spin state of the hot carriers. Our findings suggest a new approach for prolonging hot-carrier cooling in hybrid perovskites, which is conducive to further improving the performance of hot-carrier-based optoelectronic and spintronic devices.

Suggested Citation

  • Jun Yin & Rounak Naphade & Partha Maity & Luis Gutiérrez-Arzaluz & Dhaifallah Almalawi & Iman S. Roqan & Jean-Luc Brédas & Osman M. Bakr & Omar F. Mohammed, 2021. "Manipulation of hot carrier cooling dynamics in two-dimensional Dion–Jacobson hybrid perovskites via Rashba band splitting," Nature Communications, Nature, vol. 12(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-24258-7
    DOI: 10.1038/s41467-021-24258-7
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    Cited by:

    1. Gang Wang & Tanghao Liu & Bingzhe Wang & Hao Gu & Qi Wei & Zhipeng Zhang & Jun He & Mingjie Li & Guichuan Xing, 2022. "Hot-carrier tunable abnormal nonlinear absorption conversion in quasi-2D perovskite," Nature Communications, Nature, vol. 13(1), pages 1-10, December.

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