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Hidden reaction pathways inform additive engineering for perovskite LEDs

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Acknowledgements

We thank H. Zhao and C. Yuan for assistance with FLIM measurements, R. A. Kerner and J. Schwartz for helpful discussions, W. Feng for assistance with FDTD simulations, E. Ho, A. Soni and L. Wang for their assistance with optical characterization and Q. Liu and K. Wang for their helpful discussions and support. HPLC-MS measurements were performed at the Metabolite Profiling Facility, Bindley Bioscience Center, Purdue University.

Funding

This work was primarily supported by the U.S. National Science Foundation (grant nos. DMR-2539855 for materials stability and degradation mechanisms and ECCS-2552656 and ECCS-2502153 for device engineering and characterization) and the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences (grant no. DE-SC0022082 for materials synthesis and spectroscopy studies).

Author information

Author notes

  1. These authors contributed equally: Sung-Doo Baek, Yu-Ting Yang

Authors and Affiliations

  1. Davidson School of Chemical Engineering, Purdue University, West Lafayette, IN, USA

    Sung-Doo Baek, Yu-Ting Yang, Pengfei Wu, Hanjun Yang, Wenhao Shao, Jeong Hui Kim & Letian Dou

  2. Department of Chemistry, Emory University, Atlanta, GA, USA

    Sung-Doo Baek, Pengfei Wu, Xiyu Luo, Hyuntae Choi & Letian Dou

  3. Department of Chemistry, Purdue University, West Lafayette, IN, USA

    Hanjun Yang, Libai Huang & Letian Dou

  4. Department of Electrical Engineering and Computer Science, University of Michigan, Ann Arbor, MI, USA

    Mohammad Ali & L. Jay Guo

  5. Department of Physics, Princeton University, Princeton, NJ, USA

    Hui Taou Kok

  6. Department of Electrical and Computer Engineering, Princeton University, Princeton, NJ, USA

    Barry P. Rand

  7. Andlinger Center for Energy and the Environment, Princeton University, Princeton, NJ, USA

    Barry P. Rand

  8. Birck Nanotechnology Center, Purdue University, West Lafayette, IN, USA

    Letian Dou

Authors

  1. Sung-Doo Baek
  2. Yu-Ting Yang
  3. Pengfei Wu
  4. Hanjun Yang
  5. Mohammad Ali
  6. Hui Taou Kok
  7. Xiyu Luo
  8. Wenhao Shao
  9. Hyuntae Choi
  10. Jeong Hui Kim
  11. L. Jay Guo
  12. Libai Huang
  13. Barry P. Rand
  14. Letian Dou

Contributions

S.-D.B. conceived the work, designed and performed most of the experiments and developed high-performance PeLEDs. Y.-T.Y. performed the PLQY measurements, fabricated the red LEDs and participated in device optimization. P.W. synthesized 5IMAP. H.Y. and L.H. conducted the TRPL measurements. M.A. and L.J.G. performed the FDTD simulations. H.T.K. and B.P.R. conducted the angle-dependent EL measurements. X.L. fabricated the p–i–n green LEDs. J.H.K. carried out the AFM measurements. H.C. performed supporting experiments. W.S. and B.P.R. assisted with the interpretation of the results. L.D. supervised the project. S.-D.B. wrote the initial draft of the manuscript. S.-D.B., B.P.R. and L.D. revised the manuscript. All authors discussed the results and contributed to the final manuscript.

Corresponding author

Correspondence to Letian Dou.

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Competing interests

The authors declare no competing interests.

Peer review

Peer review information

Nature thanks Tae-Woo Lee and the other, anonymous, reviewer(s) for their contribution to the peer review of this work. Peer reviewer reports are available.

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Extended data figures and tables

Extended Data Fig. 1 Device characteristics under various preconditioning treatments.

a,b, EL spectra (2.5 V) (a) and EQE histograms (n = 40) (b) of devices incorporating perovskite films prepared under RT, Long-heat and Short-heat conditions.

Extended Data Fig. 2 HPLC-MS chromatograms of precursor components.

a, Total ion chromatogram. b–d, Extracted ion chromatograms of DMF ([M + H]+, m/z 74.06) (b), 2PP ([M + H]+, m/z 100.08) (c) and 5IMAP ([M + H]+, m/z 145.10) (d). The HPLC-MS analysis detected 5IMAP predominantly as a [M + H]+ ion, consistent with protonation favoured under positive-mode ESI in acidic mobile-phase conditions.

Extended Data Fig. 3 NMR spectra of synthesized 5IMAP.

a,b, 1H NMR spectrum (a) and 13C NMR spectrum (b) of 5IMAP.

Extended Data Fig. 7 Device characteristics with 4ABA, 4IMAB, 6ACA and 6IMAH.

a,b, J–V–R characteristics (a) and EQE characteristics (b) of devices based on 4ABA and 4IMAB. c,d, J–V–R characteristics (c) and EQE characteristics (d) of devices based on 6ACA and 6IMAH. The chain-length dependence (n = 4–6) may reflect spacer-length-dependent differences in defect-site coordination and precursor solubility. Both the shorter spacer (4IMAB) and the longer spacer (6IMAH) are less effective than the intermediate-length 5IMAP, probably reflecting less favourable coordination/passivation conditions. Nevertheless, all three compounds function as passivation-capable additives.

Extended Data Fig. 8 Extension of the 5IMAP strategy to red-emitting PeLEDs.

a, Normalized EL spectra of red devices (2.5 V). b, J–V–R characteristics. c, EQE characteristics. Devices incorporating 5IMAP show improved performance relative to 5AVA in a red-emitting, CsI-modified perovskite composition using the same device architecture.

Extended Data Fig. 9 Extension of the 5IMAP strategy to green-emitting PeLEDs.

a, Normalized EL spectra of green devices (2.5 V). b, J–V–L characteristics. c, EQE characteristics. Devices with 5IMAP show improved performance relative to 5AVA in FAPbBr3-based green-emitting PeLEDs.

Extended Data Fig. 10 Extension of the targeted chemical-control concept to a diamine-based additive.

a, Schematic of converting a diamine additive TTDDA into an amidinium-containing species TDAHDI through reaction with FABr. b, Device architecture. c, Normalized EL spectra (2.5 V). d, J–V–L characteristics. e, EQE characteristics. Devices incorporating TDAHDI show substantially enhanced luminance and improved EQE relative to those incorporating unreacted TTDDA.

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Baek, SD., Yang, YT., Wu, P. et al. Hidden reaction pathways inform additive engineering for perovskite LEDs. Nature 658, 629–635 (2026). https://doi.org/10.1038/s41586-026-11120-3

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