Issue

Vol. 17 (2025)

Efficient Thermally Evaporated Near-Infrared Perovskite Light-Emitting Diodes via Phase Regulation

https://doi.org/10.1007/s40820-025-01776-3
Siwei He
School of Physics and Optoelectronic Engineering, Hangzhou Institute for Advanced Study, University of Chinese Academy of Sciences, Hangzhou 310024, People’s Republic of China
Lanxin Qin
Wuhan National Laboratory for Optoelectronics (WNLO) and School of Optical and Electronic Information, Huazhong University of Science and Technology (HUST), 1037 Luoyu Road, Wuhan 430074, People’s Republic of China
Zhengzheng Liu
State Key Laboratory of Ultra‑intense Laser Science and Technology, Shanghai Institute of Optics and Fine Mechanics, Chinese Academy of Sciences, Shanghai 201800, People’s Republic of China
Jae‑Wook Kang
Department of Flexible and Printable Electronics, LANL-JBNU Engineering Institute-Korea, Jeonbuk National University, Jeonju 54896, Republic of Korea
Jiajun Luo
Wuhan National Laboratory for Optoelectronics (WNLO) and School of Optical and Electronic Information, Huazhong University of Science and Technology (HUST), 1037 Luoyu Road, Wuhan 430074, People’s Republic of China
Juan Du
School of Physics and Optoelectronic Engineering, Hangzhou Institute for Advanced Study, University of Chinese Academy of Sciences, Hangzhou 310024, People’s Republic of China

Corresponding Author: Juan Du

du@ucas.ac.cn

Nano-Micro Letters, Vol. 17 (2025), Article Number: 270

Abstract

α-phase formamidinium lead triiodide (FAPbI3) has demonstrated extraordinary properties for near-infrared perovskite light-emitting diodes (NIR-PeLEDs). The vacuum processing technique has recently received increasing attention from industry and academia due to its solvent-free feature and compatibility with large-scale production. Nevertheless, vacuum-deposited NIR-PeLEDs have been less studied, and their efficiencies lag far behind those of solution-based PeLEDs as it is still challenging to prepare pure α-FAPbI3 by the thermal evaporation. Herein, we report a Cs-containing triple-source co-evaporation approach to develop the perovskite films. The addition of thermally stable Cs cation fills in the perovskite crystal lattice and eliminates the formation of metallic Pb caused by the degradation of FA cation during the evaporation process. The tri-source co-evaporation strategy significantly promotes the phase transition from yellow δ-phase FAPbI3 to black α-phase FACsPbI3, fostering smooth, uniform, and pinhole-free perovskite films with higher crystallinity and fewer defects. On this basis, the resulting NIR-PeLED based on FACsPbI3 yields a maximum EQE of 10.25%, which is around sixfold higher than that of FAPbI3-based PeLEDs. Our work demonstrates a reliable and effective strategy to achieve α-FAPbI3 via thermal evaporation and paves the pathway toward highly efficient perovskite optoelectronic devices for future commercialization.


Highlights:
1 α-phase formamidinium lead triiodide (FAPbI3) was prepared based on triple-source co-evaporation.
2 A partial Cs-doping in the FAPbI3 can help with the suppression of the non-radiative recombination, elimination of the metallic Pb, improvement of spatial confinement.
3 Near-infrared perovskite light-emitting diodes (NIR-PeLEDs) based on triple-source co-evaporated FACsPbI3 thin films achieved a maximum external quantum efficiency of 10.25%, which was around 6 times higher than that of FAPbI3-based NIR-PeLEDs.

Keywords

Vacuum-deposited perovskite Near-infrared emission Phase regulation Co-evaporation Electroluminescence
He, Siwei, Lanxin Qin, Zhengzheng Liu, Jae‑Wook Kang, Jiajun Luo, and Juan Du. 2025. “Efficient Thermally Evaporated Near-Infrared Perovskite Light-Emitting Diodes via Phase Regulation”. Nano-Micro Letters 17 (May):270. https://doi.org/10.1007/s40820-025-01776-3.
Download Citation
Endnote/Zotero/Mendeley (RIS)
BibTeX
References
  1. X. Zhao, Z.-K. Tan, Large-area near-infrared perovskite light-emitting diodes. Nat. Photonics 14(4), 215–218 (2019). https://doi.org/10.1038/s41566-019-0559-3
  2. Y. Sun, L. Ge, L. Dai, C. Cho, J.F. Orri et al., Bright and stable perovskite light-emitting diodes in the near-infrared range. Nature 615(7954), 830–835 (2023). https://doi.org/10.1038/s41586-023-05792-4
  3. J. Li, P. Du, Q. Guo, L. Sun, Z. Shen et al., Efficient all-thermally evaporated perovskite light-emitting diodes for active-matrix displays. Nat. Photonics 17(5), 435–441 (2023). https://doi.org/10.1038/s41566-023-01177-1
  4. Y. Liu, C. Tao, Y. Cao, L. Chen, S. Wang et al., Synergistic passivation and stepped-dimensional perovskite analogs enable high-efficiency near-infrared light-emitting diodes. Nat. Commun. 13(1), 7425 (2022). https://doi.org/10.1038/s41467-022-35218-0
  5. S. He, H.B. Lee, K.-J. Ko, N. Kumar, J.-H. Jang et al., Optical engineering of FAPbBr3 nanocrystals via conjugated ligands for light-outcoupling enhancement in perovskite light-emitting diodes. Adv. Opt. Mater. 11(17), 2300486 (2023). https://doi.org/10.1002/adom.202300486
  6. Y. Liu, F. Di Stasio, C. Bi, J. Zhang, Z. Xia et al., Near-infrared light emitting metal halides: materials, mechanisms, and applications. Adv. Mater. 36(21), 2312482 (2024). https://doi.org/10.1002/adma.202312482
  7. M. Vasilopoulou, A. Fakharuddin, F.P. García de Arquer, D.G. Georgiadou, H. Kim et al., Advances in solution-processed near-infrared light-emitting diodes. Nat. Photonics 15(9), 656–669 (2021). https://doi.org/10.1038/s41566-021-00855-2
  8. Z.-L. Tseng, L.-C. Chen, L.-W. Chao, M.-J. Tsai, D. Luo et al., Aggregation control, surface passivation, and optimization of device structure toward near-infrared perovskite quantum-dot light-emitting diodes with an EQE up to 154%. Adv. Mater. 34(18), 2270132 (2022). https://doi.org/10.1002/adma.202270132
  9. J. Wei, J. Li, C. Duan, L. Yuan, S. Zou et al., High efficiency near-infrared perovskite light emitting diodes with reduced rolling-off by surface post-treatment. Small 19(20), 2207769 (2023). https://doi.org/10.1002/smll.202207769
  10. J. Luo, J. Li, L. Grater, R. Guo, A.R. Mohd Yusoff, E. Sargent, J. Tang, Vapour-deposited perovskite light-emitting diodes. Nat. Rev. Mater. 9(4), 282–294 (2024). https://doi.org/10.1038/s41578-024-00651-8
  11. P. Du, J. Li, L. Wang, L. Sun, X. Wang et al., Efficient and large-area all vacuum-deposited perovskite light-emitting diodes via spatial confinement. Nat. Commun. 12(1), 4751 (2021). https://doi.org/10.1038/s41467-021-25093-6
  12. L. Wang, J. Xu, J. Luo, W.W. Yu, Thermally evaporated perovskite light-emitting diodes for wide-color-gamut displays in AR/VR devices. Device 2(10), 100549 (2024). https://doi.org/10.1016/j.device.2024.100549
  13. Z. Zhan, Z. Liu, J. Du, S. Huang, Q. Li et al., Thermally evaporated MAPbBr3 perovskite random laser with improved speckle-free laser imaging. ACS Photonics 10(9), 3077–3086 (2023). https://doi.org/10.1021/acsphotonics.3c00435
  14. Y. Hu, Q. Wang, Y.-L. Shi, M. Li, L. Zhang et al., Vacuum-evaporated all-inorganic cesium lead bromine perovskites for high-performance light-emitting diodes. J. Mater. Chem. C 5(32), 8144–8149 (2017). https://doi.org/10.1039/C7TC02477K
  15. X. Lian, X. Wang, Y. Ling, E. Lochner, L. Tan et al., Light emitting diodes based on inorganic composite halide perovskites. Adv. Funct. Mater. 29(5), 1807345 (2019). https://doi.org/10.1002/adfm.201807345
  16. C. Chen, T.-H. Han, S. Tan, J. Xue, Y. Zhao et al., Efficient flexible inorganic perovskite light-emitting diodes fabricated with CsPbBr3 emitters prepared via low-temperature in situ dynamic thermal crystallization. Nano Lett. 20(6), 4673–4680 (2020). https://doi.org/10.1021/acs.nanolett.0c01550
  17. C.-A. Hsieh, G.-H. Tan, Y.-T. Chuang, H.-C. Lin, P.-T. Lai et al., Vacuum-deposited inorganic perovskite light-emitting diodes with external quantum efficiency exceeding 10% via composition and crystallinity manipulation of emission layer under high vacuum. Adv. Sci. 10(10), 2206076 (2023). https://doi.org/10.1002/advs.202206076
  18. J. Li, P. Du, S. Li, J. Liu, M. Zhu et al., High-throughput combinatorial optimizations of perovskite light-emitting diodes based on all-vacuum deposition. Adv. Funct. Mater. 29(51), 1903607 (2019). https://doi.org/10.1002/adfm.201903607
  19. B. Dänekamp, N. Droseros, F. Palazon, M. Sessolo, N. Banerji et al., Efficient photo- and electroluminescence by trap states passivation in vacuum-deposited hybrid perovskite thin films. ACS Appl. Mater. Interfaces 10(42), 36187–36193 (2018). https://doi.org/10.1021/acsami.8b13100
  20. J. Borchert, R.L. Milot, J.B. Patel, C.L. Davies, A.D. Wright et al., Large-area, highly uniform evaporated formamidinium lead triiodide thin films for solar cells. ACS Energy Lett. 2(12), 2799–2804 (2017). https://doi.org/10.1021/acsenergylett.7b00967
  21. D. Lin, Y. Gao, T. Zhang, Z. Zhan, N. Pang et al., Vapor deposited pure α-FAPbI3 perovskite solar cell via moisture-induced phase transition strategy. Adv. Funct. Mater. 32(48), 2208392 (2022). https://doi.org/10.1002/adfm.202208392
  22. M. Kroll, S.D. Öz, Z. Zhang, R. Ji, T. Schramm et al., Insights into the evaporation behaviour of FAI: material degradation and consequences for perovskite solar cells. Sustain. Energy Fuels 6(13), 3230–3239 (2022). https://doi.org/10.1039/D2SE00373B
  23. A.-F. Castro-Méndez, F. Jahanbakhshi, D.K. LaFollette, B.J. Lawrie, R. Li et al., Tailoring interface energies via phosphonic acids to grow and stabilize cubic FAPbI3 deposited by thermal evaporation. J. Am. Chem. Soc. 146(27), 18459–18469 (2024). https://doi.org/10.1021/jacs.4c03911
  24. Z. Yuan, Y. Miao, Z. Hu, W. Xu, C. Kuang et al., Unveiling the synergistic effect of precursor stoichiometry and interfacial reactions for perovskite light-emitting diodes. Nat. Commun. 10(1), 2818 (2019). https://doi.org/10.1038/s41467-019-10612-3
  25. B.-W. Park, H.W. Kwon, Y. Lee, D.Y. Lee, M.G. Kim et al., Stabilization of formamidinium lead triiodide α-phase with isopropylammonium chloride for perovskite solar cells. Nat. Energy 6(4), 419–428 (2021). https://doi.org/10.1038/s41560-021-00802-z
  26. J.-W. Lee, D.-H. Kim, H.-S. Kim, S.-W. Seo, S.M. Cho et al., Formamidinium and cesium hybridization for photo- and moisture-stable perovskite solar cell. Adv. Energy Mater. 5(20), 1501310 (2015). https://doi.org/10.1002/aenm.201501310
  27. M. Saliba, T. Matsui, J.-Y. Seo, K. Domanski, J.-P. Correa-Baena et al., Cesium-containing triple cation perovskite solar cells: improved stability, reproducibility and high efficiency. Energy Environ. Sci. 9(6), 1989–1997 (2016). https://doi.org/10.1039/C5EE03874J
  28. Z. Li, M. Yang, J.-S. Park, S.-H. Wei, J.J. Berry et al., Stabilizing perovskite structures by tuning tolerance factor: formation of formamidinium and cesium lead iodide solid-state alloys. Chem. Mater. 28(1), 284–292 (2016). https://doi.org/10.1021/acs.chemmater.5b04107
  29. K.A. Elmestekawy, A.D. Wright, K.B. Lohmann, J. Borchert, M.B. Johnston et al., Controlling intrinsic quantum confinement in formamidinium lead triiodide perovskite through Cs substitution. ACS Nano 16(6), 9640–9650 (2022). https://doi.org/10.1021/acsnano.2c02970
  30. L. Gil-Escrig, C. Momblona, M.-G. La-Placa, P.P. Boix, M. Sessolo et al., Vacuum deposited triple-cation mixed-halide perovskite solar cells. Adv. Energy Mater. 8(14), 1703506 (2018). https://doi.org/10.1002/aenm.201703506
  31. H.B. Lee, R. Sahani, V. Devaraj, N. Kumar, B. Tyagi et al., Complex additive-assisted crystal growth and phase stabilization of α-FAPbI3 film for highly efficient, air-stable perovskite photovoltaics. Adv. Mater. Interfaces 10(2), 2201658 (2023). https://doi.org/10.1002/admi.202201658
  32. B. Guo, R. Lai, S. Jiang, L. Zhou, Z. Ren et al., Ultrastable near-infrared perovskite light-emitting diodes. Nat. Photonics 16(9), 637–643 (2022). https://doi.org/10.1038/s41566-022-01046-3
  33. G. Rainò, N. Yazdani, S.C. Boehme, M. Kober-Czerny, C. Zhu et al., Ultra-narrow room-temperature emission from single CsPbBr3 perovskite quantum dots. Nat. Commun. 13(1), 2587 (2022). https://doi.org/10.1038/s41467-022-30016-0
  34. D. Bi, C. Yi, J. Luo, J.-D. Décoppet, F. Zhang et al., Polymer-templated nucleation and crystal growth of perovskite films for solar cells with efficiency greater than 21%. Nat. Energy 1, 16142 (2016). https://doi.org/10.1038/nenergy.2016.142
  35. S. Ding, M. Hao, C. Fu, T. Lin, A. Baktash et al., In situ bonding regulation of surface ligands for efficient and stable FAPbI3 quantum dot solar cells. Adv. Sci. 9(35), 2204476 (2022). https://doi.org/10.1002/advs.202204476
  36. R. Lindblad, N.K. Jena, B. Philippe, J. Oscarsson, D. Bi et al., Electronic structure of CH3NH3PbX3 perovskites: dependence on the halide moiety. J. Phys. Chem. C 119(4), 1818–1825 (2015). https://doi.org/10.1021/jp509460h
  37. Z. Zhu, J. Ma, Z. Wang, C. Mu, Z. Fan et al., Efficiency enhancement of perovskite solar cells through fast electron extraction: the role of graphene quantum dots. J. Am. Chem. Soc. 136(10), 3760–3763 (2014). https://doi.org/10.1021/ja4132246
  38. H. Wang, X. Zhang, Q. Wu, F. Cao, D. Yang et al., Trifluoroacetate induced small-grained CsPbBr3 perovskite films result in efficient and stable light-emitting devices. Nat. Commun. 10(1), 665 (2019). https://doi.org/10.1038/s41467-019-08425-5
  39. M. Liu, O. Voznyy, R. Sabatini, F.P. García de Arquer, R. Munir et al., Hybrid organic-inorganic inks flatten the energy landscape in colloidal quantum dot solids. Nat. Mater. 16(2), 258–263 (2017). https://doi.org/10.1038/nmat4800
  40. D. Han, J. Wang, L. Agosta, Z. Zang, B. Zhao et al., Tautomeric mixture coordination enables efficient lead-free perovskite LEDs. Nature 622(7983), 493–498 (2023). https://doi.org/10.1038/s41586-023-06514-6
  41. J. Fu, Q. Xu, G. Han, B. Wu, C.H.A. Huan et al., Hot carrier cooling mechanisms in halide perovskites. Nat. Commun. 8(1), 1300 (2017). https://doi.org/10.1038/s41467-017-01360-3
  42. S.G. Motti, D. Meggiolaro, S. Martani, R. Sorrentino, A.J. Barker et al., Defect activity in lead halide perovskites. Adv. Mater. 31(47), 1901183 (2019). https://doi.org/10.1002/adma.201901183
  43. A.-F. Castro-Méndez, J. Hidalgo, J.-P. Correa-Baena, The role of grain boundaries in perovskite solar cells. Adv. Energy Mater. 9(38), 1901489 (2019). https://doi.org/10.1002/aenm.201901489
  44. L. Xu, J. Li, B. Cai, J. Song, F. Zhang et al., A bilateral interfacial passivation strategy promoting efficiency and stability of perovskite quantum dot light-emitting diodes. Nat. Commun. 11(1), 3902 (2020). https://doi.org/10.1038/s41467-020-17633-3
  45. S. He, N. Kumar, H.B. Lee, K.-J. Ko, Y.-J. Jung et al., Tailoring the refractive index and surface defects of CsPbBr3 quantum dots via alkyl cation-engineering for efficient perovskite light-emitting diodes. Chem. Eng. J. 425, 130678 (2021). https://doi.org/10.1016/j.cej.2021.130678
  46. Y. Miao, Y. Ke, N. Wang, W. Zou, M. Xu et al., Stable and bright formamidinium-based perovskite light-emitting diodes with high energy conversion efficiency. Nat. Commun. 10(1), 3624 (2019). https://doi.org/10.1038/s41467-019-11567-1
  47. Y. Ji, Q. Zhong, M. Yu, H. Yan, L. Li et al., Amphoteric chelating ultrasmall colloids for FAPbI3 nanodomains enable efficient near-infrared light-emitting diodes. ACS Nano 18(11), 8157–8167 (2024). https://doi.org/10.1021/acsnano.3c11941
Read More
Author biographies are not available.
Download this PDF file
PDF SUPPLEMENTARY FILE
Statistic
Read Counter : 1445 Download : 1076

Most read articles by the same author(s)