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Gigantic suppression of recombination rate in 3D lead-halide perovskites for enhanced photodetector performance

Nature Photonics volume 17, pages 236–243 (2023)Cite this article

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Abstract

Prolonging the carrier lifetime in lead-halide perovskite (LHP) can enable novel schemes for highly efficient energy-harvesting and photodetection applications. However, suppressing the recombination processes in LHP without chemical treatments remains an open challenge. Here we show that the recombination rate of three-dimensional LHP polycrystalline thin films can decrease significantly when placed on hyperbolic metamaterials. Through momentum-resolved imaging, we reveal that these LHP films possess a dominant in-plane transition dipole, which in turn is responsible for the decrease in the recombination rate. We observe a decrease in the recombination rate of a MAPbI3 LHP thin film by ~50% and 30% when placed on a plasmonic mirror and a hyperbolic metamaterial, respectively. Furthermore, we discover a tenfold decrease in the recombination rate of (Cs0.06FA0.79MA0.15)Pb(I0.85Br0.15)3, and the origin of this giant reduction in the recombination process is discussed based on exciton-trapping dynamics. By controlling the recombination rate of LHPs, we demonstrate a 250% increase in photoresponsivity of LHP-based photodetectors. The resulting physical insights will provide novel means to enhance the efficiency of LHP-based optoelectronic and photonic devices.

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Fig. 1: Purcell effect of an anisotropic transition dipole in the presence of a plasmonic substrate.
Fig. 2: Momentum-resolved radiation and TRPL measurements of MAPbI3 and LDS750 films.
Fig. 3: TRPL results of MAPbBr3 and DCM films.
Fig. 4: TRPL results for the TCLHP ((Cs0.06FA0.79MA0.15) Pb(I0.85Br0.15)3) film and a schematic illustration of the relevant recombination processes.
Fig. 5: Enhancement of recombination time.
Fig. 6: Enhanced photoresponsivity of LHPs with suppressed recombination rate.

Data availability

The data that support the findings of this study are available from the corresponding author upon reasonable request.

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Acknowledgements

This research was supported by the Bill and Melinda Gates Foundation, the Army Research Office, the National Science Foundation and the National Natural Science Foundation.

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Author notes

  1. Kwang Jin Lee

    Present address: Center for Molecular Spectroscopy and Dynamics, Institute for Basic Science (IBS), Seoul, Republic of Korea

  2. Jihua Zhang

    Present address: ARC Centre of Excellence for Transformative Meta-Optical Systems (TMOS), Research School of Physics, The Australian National University, Canberra, Australia

  3. Mohamed ElKabbash

    Present address: Research Laboratory of Electronics, MIT, Cambridge, MA, USA

Authors and Affiliations

  1. The Institute of Optics, University of Rochester, Rochester, NY, USA

    Kwang Jin Lee, Ran Wei, Jihua Zhang, Mohamed ElKabbash & Chunlei Guo

  2. GPL, Changchun Institute of Optics, Fine Mechanics and Physics, Chinese Academy of Sciences, Changchun, China

    Ye Wang, Wenchi Kong, Sandeep Kumar Chamoli, Tao Huang & Weili Yu

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Contributions

K.J.L., M.E. and C.G. discussed and defined the project. K.J.L. and M.E. initiated the project and designed and coordinated the experiments. Y.W. characterized the optical properties of the samples. R.W. prepared the nanophotonic substrates and performed numerical calculations of absorption. K.J.L. and Y.W. performed TRPL measurements. K.J.L. and J.Z. carried out the radiation pattern measurements. S.K.C. and M.E. performed the Purcell factor calculations. W.K., T.H. and W.Y. carried out the photodetector experiment. K.J.L., M.E. and C.G. analysed the data. K.J.L., M.E. and C.G. wrote the manuscript. C.G. supervised the overall project. All authors commented on the paper.

Corresponding authors

Correspondence to Kwang Jin Lee, Mohamed ElKabbash or Chunlei Guo.

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Nature Photonics thanks Takashi Asano, Matthew Pelton and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary Figs. 1–18, notes I–VII and Tables 1–5.

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Lee, K.J., Wei, R., Wang, Y. et al. Gigantic suppression of recombination rate in 3D lead-halide perovskites for enhanced photodetector performance. Nat. Photon. 17, 236–243 (2023). https://doi.org/10.1038/s41566-022-01151-3

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