Surface-binding molecular multipods strengthen the halide perovskite lattice and boost luminescence

Dong Hyeok Kim; Seung Je Woo; Claudia Pereyra Huelmo; Min Ho Park; Aaron M. Schankler; Zhenbang Dai; Jung Min Heo; Sungjin Kim; Guy Reuveni; Sungsu Kang; Joo Sung Kim; Hyung Joong Yun; Jinwoo Park; Jungwon Park; Omer Yaffe; Andrew M. Rappe; Tae Woo Lee

doi:10.1038/s41467-024-49751-7

Surface-binding molecular multipods strengthen the halide perovskite lattice and boost luminescence

Dong Hyeok Kim, Seung Je Woo, Claudia Pereyra Huelmo, Min Ho Park, Aaron M. Schankler, Zhenbang Dai, Jung Min Heo, Sungjin Kim, Guy Reuveni, Sungsu Kang, Joo Sung Kim, Hyung Joong Yun, Jinwoo Park, Jungwon Park, Omer Yaffe, Andrew M. Rappe^*, Tae Woo Lee^*

^*Corresponding author for this work

Department of Chemical and Biological Physics

Research output: Contribution to journal › Article › peer-review

4 Citations (Scopus)

Abstract

Reducing the size of perovskite crystals to confine excitons and passivating surface defects has fueled a significant advance in the luminescence efficiency of perovskite light-emitting diodes (LEDs). However, the persistent gap between the optical limit of electroluminescence efficiency and the photoluminescence efficiency of colloidal perovskite nanocrystals (PeNCs) suggests that defect passivation alone is not sufficient to achieve highly efficient colloidal PeNC-LEDs. Here, we present a materials approach to controlling the dynamic nature of the perovskite surface. Our experimental and theoretical studies reveal that conjugated molecular multipods (CMMs) adsorb onto the perovskite surface by multipodal hydrogen bonding and van der Waals interactions, strengthening the near-surface perovskite lattice and reducing ionic fluctuations which are related to nonradiative recombination. The CMM treatment strengthens the perovskite lattice and suppresses its dynamic disorder, resulting in a near-unity photoluminescence quantum yield of PeNC films and a high external quantum efficiency (26.1%) of PeNC-LED with pure green emission that matches the Rec.2020 color standard for next-generation vivid displays.

Original language	English
Article number	6245
Number of pages	12
Journal	Nature Communications
Volume	15
Early online date	24 Jul 2024
DOIs	https://doi.org/10.1038/s41467-024-49751-7
Publication status	Published - 24 Jul 2024

Funding

This work was supported by the National Research Foundation of Korea (NRF) grant funded by the Ministry of Science and ICT (MSIT) (NRF-2016R1A3B1908431) and NRF grant Brain Link program (2022H1D3A3A01081288). The first-principles DFT modeling of CMM-perovskite interactions with FAPbBr3 and (FA1−xGAx)PbBr3, elasticity calculations, and corresponding AIMD simulations for TPBi CMM, and all isolated CMM calculations were conducted by C.P.H. under the support of the NSF Center for Integration of Modern Optoelectronic Materials on Demand (IMOD), an NSF Science and Technology Center (STC) supported by NSF grant DMR-2019444. The first-principles DFT modeling of CMM-perovskite interactions with FAPbBr3, elasticity calculations, and corresponding AIMD simulations for PO-T2T and 3TPYMB CMMs, were conducted by A.M.S., Z.D., and A.M.R. under support from the U.S. Department of Energy, Office of Science, Basic Energy Sciences, under award no. DE-FG02-07ER46431. Computational support was provided by the National Energy Research Scientific Computing Center (NERSC), a U.S. Department of Energy, Office of Science User Facility located at Lawrence Berkeley National Laboratory, operated under contract no. DE-AC02-05CH11231. Publisher Copyright: © The Author(s) 2024.

All Science Journal Classification (ASJC) codes

General Chemistry
General Biochemistry,Genetics and Molecular Biology
General Physics and Astronomy

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Cite this

Kim, D. H., Woo, S. J., Huelmo, C. P., Park, M. H., Schankler, A. M., Dai, Z., Heo, J. M., Kim, S., Reuveni, G., Kang, S., Kim, J. S., Yun, H. J., Park, J., Park, J., Yaffe, O., Rappe, A. M., & Lee, T. W. (2024). Surface-binding molecular multipods strengthen the halide perovskite lattice and boost luminescence. Nature Communications, 15, Article 6245. https://doi.org/10.1038/s41467-024-49751-7

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abstract = "Reducing the size of perovskite crystals to confine excitons and passivating surface defects has fueled a significant advance in the luminescence efficiency of perovskite light-emitting diodes (LEDs). However, the persistent gap between the optical limit of electroluminescence efficiency and the photoluminescence efficiency of colloidal perovskite nanocrystals (PeNCs) suggests that defect passivation alone is not sufficient to achieve highly efficient colloidal PeNC-LEDs. Here, we present a materials approach to controlling the dynamic nature of the perovskite surface. Our experimental and theoretical studies reveal that conjugated molecular multipods (CMMs) adsorb onto the perovskite surface by multipodal hydrogen bonding and van der Waals interactions, strengthening the near-surface perovskite lattice and reducing ionic fluctuations which are related to nonradiative recombination. The CMM treatment strengthens the perovskite lattice and suppresses its dynamic disorder, resulting in a near-unity photoluminescence quantum yield of PeNC films and a high external quantum efficiency (26.1%) of PeNC-LED with pure green emission that matches the Rec.2020 color standard for next-generation vivid displays.",

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AU - Schankler, Aaron M.

AU - Dai, Zhenbang

AU - Heo, Jung Min

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AU - Reuveni, Guy

AU - Kang, Sungsu

AU - Kim, Joo Sung

AU - Yun, Hyung Joong

AU - Park, Jinwoo

AU - Park, Jungwon

AU - Yaffe, Omer

AU - Rappe, Andrew M.

AU - Lee, Tae Woo

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Surface-binding molecular multipods strengthen the halide perovskite lattice and boost luminescence

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