Abstract
Metal halide perovskite light-emitting diodes (PeLEDs) have demonstrated excellent external quantum efficiency (EQE), easy colour tunability and low-cost processability, making them promising next-generation display techniques1,2,3. However, PeLEDs still underperform compared with organic light-emitting diodes (LEDs) with an EQE of about 40% because of insufficient charge confinement and defect-caused non-radiative recombination on the film surface. Here we report a spontaneously formed 3D/2D vertically oriented perovskite heterojunction by means of a simple one-step spin-coating method, which could effectively confine the charge carriers and shift the radiation zone away from the defect-rich surface region. Notably, the 2D perovskite on top exhibits a wrinkled surface morphology, which offers up to 45.4% light extraction efficiency. The resulting PeLEDs achieved an EQE of 42.9% for the green emission (certified 42.3%). Our work sheds light on the strategies for fabricating high-efficiency PeLEDs in the future.
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The data that support the findings of this study are fully and freely available from the corresponding authors. Source data are provided with this paper.
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Acknowledgements
This work was supported by the programme of the National Natural Science Foundation of China (nos. 12274173, 62574097, 12374375 and 12172598), the Science and Technology Development Project of Jilin Province (20240101008JJ), Fudan University Talent Introduction Project, Beijing Natural Science Foundation (Z220007) and Fundamental and Interdisciplinary Disciplines Breakthrough Plan of the Ministry of Education of China. We thank the accelerator scientists and the staff of beamlines BL02U2, BL19U2, BL17B1 and BL06B at SSRF for providing the beam time and the User Experiment Assist System at SSRF for their help. We also acknowledge the instrument and equipment sharing platform of the College of Physics, Jilin University, for access to SEM, X-ray diffraction, XPS and TRPL measurements. Y.Y. and S.F. acknowledge the support of the Electron Microscopy Platform of the Shanghai Institute of Applied Physics, Chinese Academy of Sciences. We thank X. Bai, Y. Zhang, Y. Liu and Z. Yuan for discussions.
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W.J. conceived the central idea and concept. Y.Y., H.L., A.T and W.X. supervised the work. J.P., X.X. and S.L. carried out device fabrication and characterizations, with the assistance of T.Y. and B.Z. H.Z. and X.W. provided noteworthy analyses. G.C., S.F., L.L., R.T. and Y.Y. carried out TEM and GIWAXS measurements and provided analyses. J.P. and X.X. carried out optical simulations of the device and perovskite films. W.J. and S.L. co-wrote the paper and Y.Y. and H.L. provided substantial revisions. All authors discussed the results and commented on the manuscript.
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Extended data figures and tables
Extended Data Fig. 1 Characterization of interactions between PVK, PEIE and perovskite films.
a, 1D GIWAXS patterns of PVK film on ITO substrate. Inset, an enlarged view of the region in the green circle in Fig. 1a, showing a distinct diffraction peak. b, FTIR spectra of PVK, PEIE and PVK/PEIE. The OH stretching peak of PEIE shifts by 73.5 cm−1 after reacting with PVK, indicating the formation of hydrogen bonds between PEIE and the PVK layer. c, 1D GIWAXS patterns of PVK/PEIE film on ITO substrate. d, FTIR spectra of PVK/PEIE, pure perovskite on glass substrate and target perovskite. The peak at 1,043.3 cm−1, attributed to the C–O bond, shifts to a lower wavenumber after reacting with the perovskite, suggesting a chemical interaction between PEIE and Pb2+ ions in the perovskite. e, Photographs of PEABr, FABr and PbBr2 DMSO solution after dropping the PEIE solution. f, XPS spectra of Pb 4f. For the XPS measurements, perovskite precursors were spin coated on the PVK and PVK/PEIE substrates and then rinsed with DMSO to confirm the coordination interaction between PEIE and Pb2+ ions.
Extended Data Fig. 2 Analysis and mapping of cross-sectional morphology and lead distribution in perovskite films.
Cross-sectional TEM images and corresponding Pb elemental mapping for both control and target perovskite films. The control film reveals uniform contrast and a homogeneous spatial distribution of Pb, consistent with a randomly mixed phase. By contrast, the target film exhibits pronounced spatial heterogeneity in Pb distribution. Specifically, the Pb signal intensity decreases near the top interface, attributable to a higher proportion of 2D perovskite and an increased density of spacer molecules in the upper region. To aid interpretation, the TEM images were subjected to binary processing using ImageJ. The distinct contrast further corroborates the well-defined heterojunction architecture in the target film, as opposed to the randomly distributed phases observed in the control sample.
Extended Data Fig. 3 Characterization of crystallization and growth of perovskite films.
a,b, 2D GIWAXS patterns during the spin-coating process of control (a) and target (b) perovskite films sequentially show ten distinct time points, ranging from 5 s to 68 s, with each image captured at 7-s intervals.
Extended Data Fig. 4 Surface morphology of perovskite films.
a,b, AFM height images of control (a) and target (b) perovskite films.
Extended Data Fig. 5 Energy-level properties of perovskite films.
a, UPS spectra showing high-binding-energy secondary-electron cut-off (left) and valence band (VB) edge regions (right) of control and target films. b, Conduction band (CB) and VB energy levels of 3D and 2D phases.
Extended Data Fig. 6 Electron transport properties in the devices.
a, J–V–L curves of PeLEDs fabricated on PVK/PEIE with different ETLs. PO-T2T (2,4,6-tris[3-(diphenylphosphinyl)phenyl]-1,3,5-triazine) exhibits higher electron mobility than B3PyMPM. Devices with PO-T2T as the ETL show higher current density, indicating that electron injection and transport are limited primarily by the organic ETL rather than the perovskite layer. b, Transient EL response of control and target PeLEDs under a 2.8 V pulsed bias. The target device shows a longer delay time (ttarget, between the voltage pulse and EL onset) compared with the control device. Because EL onset is governed by the transit of minor carriers, the prolonged ttarget indicates slower electron transport from the cathode to the emissive layer in the target device. c, Schematic diagram illustrating the relationship between electron transport and EL onset. In the control device, excitons form predominantly at the perovskite–ETL interface and the delay time (tcontrol) is limited by electron transit across the B3PyMPM layer. By contrast, in the target device, excitons form mainly at the 3D/2D perovskite heterojunction, farther from the ETL interface. Thus, ttarget is governed by electron transport across both the B3PyMPM and the 2D perovskite layer.
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Peng, J., Xue, X., Liu, S. et al. Maximizing perovskite electroluminescence with ordered 3D/2D heterojunction. Nature 651, 76–82 (2026). https://doi.org/10.1038/s41586-026-10134-1
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DOI: https://doi.org/10.1038/s41586-026-10134-1


