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Multiple exciton generation in tin–lead halide perovskite nanocrystals for photocurrent quantum efficiency enhancement

Nature Photonics volume 16, pages 485–490 (2022)Cite this article

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Abstract

Multiple exciton generation (MEG), the generation of multiple electron–hole pairs from a single high-energy photon, can enhance the photoconversion efficiency in several technologies including photovoltaics, photon detection and solar-fuel production1,2,3,4,5,6. However, low efficiency, high photon-energy threshold and fast Auger recombination impede its practical application1,7. Here we achieve enhanced MEG with an efficiency of up to 87% and photon-energy threshold of two times the bandgap in highly stable, weakly confined formamidinium tin–lead iodide perovskite nanocrystals (FAPb1–xSnxI3 NCs; x ≤ 0.11). Importantly, an MEG-driven increment in the internal photocurrent quantum efficiency exceeding 100% with a low threshold is observed in such NC-sensitized photoconductors under ultraviolet-light illumination. The MEG enhancement mechanism is found to be mediated by the slower cooling and reduced trapping of hot carriers above the MEG threshold after the partial substitution of Pb by Sn. Our findings corroborate the potential importance of narrow-bandgap perovskite NCs for the development of optoelectronics that could benefit from MEG.

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Fig. 1: Efficient MEG in FAPb1–xSnxI3 NCs.
Fig. 2: Enhanced photocurrent conversion efficiency by MEG in FAPb1–xSnxI3 NCs.
Fig. 3: Roles of hot-carrier cooling and trapping on MEG.
Fig. 4: Calculations of hot-carrier relaxation dynamics and defects formation.

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Data availability

All data supporting the findings of this study are present in this Letter and its Supplementary Information. Additional data are available from the corresponding authors upon reasonable request.

Code availability

The codes used in this study are available from the corresponding authors upon reasonable request.

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  • 31 May 2022

    In the version of this article initially published, the second affiliation omitted institutional divisions, which have now been restored to the HTML and PDF versions of the article.

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Acknowledgements

M.L. acknowledges financial support from the Hong Kong Polytechnic University (grants 1-BE2Z, W188 and 1-ZVGH) and the Shenzhen Science, Technology and Innovation Commission (project no. R2021A064). J.Y., O.M.B. and O.F.M. acknowledge the Supercomputing Laboratory at KAUST for their efficient technical assistance.

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Author notes

  1. These authors contributed equally: Yifan Chen, Jun Yin.

Authors and Affiliations

  1. Department of Applied Physics, The Hong Kong Polytechnic University, Hong Kong, China

    Yifan Chen, Qi Wei, Chenhao Wang, Xiaoting Wang, Hui Ren, Siu Fung Yu & Mingjie Li

  2. Advanced Membranes and Porous Materials Center, KAUST Catalysis Center, Physical Science and Engineering Division, King Abdullah University of Science and Technology (KAUST), Thuwal, Kingdom of Saudi Arabia

    Jun Yin, Osman M. Bakr & Omar F. Mohammed

  3. The Hong Kong Polytechnic University Shenzhen Research Institute, Shenzhen, People’s Republic of China

    Mingjie Li

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  1. Yifan Chen
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Contributions

M.L. conceived the idea and designed the experiments. Y.C. performed the sample and device fabrications, characterizations and optical/electrical measurements. M.L., Y.C. and Q.W. performed the TA and TRPL measurements. C.W., X.W. and H.R. assisted in sample fabrications and characterizations. J.Y., O.M.B. and O.F.M. performed the DFT and NAMD calculations. M.L., Y.C., J.Y. and O.F.M. drafted the manuscript. S.F.Y. assisted in interpreting the results and drafting the manuscript. All the authors discussed the results and commented on the manuscript at all stages.

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Correspondence to Omar F. Mohammed or Mingjie Li.

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Nature Photonics thanks Nathaniel Gabor, Bruce Parkinson and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary Notes 1–3, Table 1 and Figs. 1–27.

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Chen, Y., Yin, J., Wei, Q. et al. Multiple exciton generation in tin–lead halide perovskite nanocrystals for photocurrent quantum efficiency enhancement. Nat. Photon. 16, 485–490 (2022). https://doi.org/10.1038/s41566-022-01006-x

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