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Local lattice softening in semiconductor quantum dots for efficient white light-emitting diodes

Abstract

White light-emitting diodes based on single-component quantum dots (sc-WQLEDs) have gained great attention owing to their low operating voltage and the high spectral stability of their emission. However, their performance presently lags far behind that of state-of-the-art white organic LEDs owing to a lack of efficient white quantum dot emitters. Creating self-trapped excitons in semiconductor quantum dots is a promising approach to producing broadband white emission. However, such emitters generally suffer from poor charge transport and structural instability. Here we accomplish controllable synthesis of core/shell structured ZnSe/ZnS quantum dots with efficient white emission through combining a sharp excitonic blue emission with a broadband yellow self-trapped exciton emission owing to local lattice softening of ZnSe cores by heterovalent doping with halogen ions. We reveal that the self-trapped excitons confined in the surrounding ZnSe covalent-bond matrix can generate strong and stable yellow emission with minimal reduction of the excitonic blue emission and charge transport capability of ZnSe. On the basis of this approach, we demonstrate highly efficient, heavy-metal-free WQLEDs with a maximum external quantum efficiency up to 15% (average 10.5 ± 2.6%), a luminance of over 26,000 cd m2 as well as exceptional device operational lifetime with T50 exceeding 2,500 h at an initial luminance of 100 cd m2.

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Fig. 1: Preparation and structural analysis of the white QDs.
Fig. 2: Luminescence mechanism and optical properties of white QDs.
Fig. 3: Ultrafast exciton dynamics and band structure of white QDs.
Fig. 4: Device structure and performance of sc-WQLEDs.

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Data availability

The data supporting the findings of this study are available within the article and its Supplementary Information. The source data files are available via figshare at https://doi.org/10.6084/m9.figshare.29107793.v1 (ref. 60). Source data are provided with this paper.

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Acknowledgements

X.Y. acknowledges financial support from the National Key Research and Development Program of China (project 2022YFB3602902 and 2024YFB3612404), the National Natural Science Foundation of China (62174104), the Shanghai Science and Technology Committee (19010500600), and the Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning. G.J. acknowledges the Australian Research Council (ARC) Future Fellowship Scheme (FT210100509). S.S. and X.G. acknowledge funding support from the University of Michigan and NSF grant #DMR-1625671. L.D. acknowledges funding support from UKRI Horizon Europe Guarantee MSCA Marie Skłodowska-Curie Postdoctoral Fellowship (EP/Y029429/1). S.D.S. acknowledges the Royal Society and Tata Group (grant numbers UF150033, URF\R\221026). L.D. and S.D.S acknowledge the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (HYPERION, grant agreement no. 756962).

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Contributions

X.Y. conceived the idea and guided the whole project. S.W. designed and performed most of the experiments, analysed the data and wrote the paper. C.W., B.L. and L.D. carried out the TA and PDS, analysed the data and helped in paper writing. Y.W. and H.W. helped with the material synthesis and characterization. T.L. contributed to the device optimization. H.S. and W.Z. performed the HAADF-STEM measurement. C.W. and Z.L. contributed to the DFT calculations under supervision from G.Z. Jiayi Chen contributed to element mapping under supervision from G.J. S.S. analysed the temperature-dependent PL data. X.Y., X.G., Q.W., Jianhua Zhang, L.D., B.L., G.J., L.W., Jun Chen, X.B., Jiaqi Zhang, S.D.S. and R.H.F. prepared and polished the paper. All authors contributed to the discussion and review of the paper.

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Correspondence to Jianhua Zhang, Xiwen Gong or Xuyong Yang.

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Nature Photonics thanks Eunjoo Jang and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Extended data

Extended Data Table 1 Huang-Rhys factors of some compounds
Extended Data Table 2 Summary of recently reported sc-WQLEDs showing emission characteristics and stability (lifetime)

Extended Data Fig. 1 Local lattice softening in Cl:ZnSe.

a, b, Comparison of the equilibrium geometric structures of pristine ZnSe between (a) GS and (b) ES. c, d, Comparison of equilibrium geometric structures near ClSe-VZn2− region of Cl:ZnSe between (c) GS and (d) ES. Upon photoexcitation, the Cl-Cl and Se-Se bond contract.

Extended Data Fig. 2 Exciton distribution variations induced by local soft lattices in ES.

Exciton density distributions for a, ZnSe and b, Cl:ZnSe.

Extended Data Fig. 3 Characterization for single-component white emissions.

a, PL mapping of Cl:ZnSe/ZnSe/ZnS QDs using filters of 420-480 nm and 495-550 nm, respectively. These filters enable the detection of emission occurring within their respective wavelength ranges. The individual QDs (circled in green) exhibit distinct bright dots under both filters, indicating that the white emissions originate from the same particle. b, PL intensity time trace of Cl:ZnSe/ZnSe/ZnS QDs for the two emissions detected by the aforementioned filters, respectively. The non-blinking behavior observed for each emission peak suggests the effective suppression of Auger combination process. The excited wavelength used is 405 nm. c, Photoluminescence excitation (PLE) spectra of Cl:ZnSe/ZnSe/ZnS QDs with different PL wavelengths covering the entire PL spectra. These PLE spectral profiles are almost identical, which rule out the possibility that the multiple emissions result from the radiation ensemble of different emitters. This observation is consistent with the fact that the optimal excitation wavelength varies for different materials. Any other scenario would result in a variation in the excitation spectrum with changes in the detection wavelength. d, PL spectra of Cl:ZnSe/ZnSe/ZnS QDs under varying excitation light. The insert provides a zoom-in view of the low-energy emission region under excitation wavelengths ranging from 470 to 650 nm. It is discernible that the broadband emissions vanish when the excitation wavelengths exceed 500 nm, illustrating that the low-energy emission is dependent on the energy or charge transfer from ZnSe host.

Source data

Extended Data Fig. 4 Temperature-dependent PL measurement.

2D colour map of temperature-dependent PL spectra of a, pristine ZnSe/ZnS QDs and b, Cl:ZnSe/ZnSe/ZnS QDs, respectively. The temperature stable PL emissions of Cl doped QDs may result from a combined effect of reduced thermal expansion and enhanced energy transfer from the FE to the STE states.

Source data

Extended Data Fig. 5 Performance of the champion sc-WQLED.

a, J-V-L and b, L-EQE characteristics. Inset shows the EL spectrum of the device.

Source data

Supplementary information

Supplementary Information

Supplementary Figs. 1–22 and Tables 1–3.

Source data

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Source Data Extended Data Fig. 3

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Wang, S., Wang, C., Wang, Y. et al. Local lattice softening in semiconductor quantum dots for efficient white light-emitting diodes. Nat. Photon. 19, 952–959 (2025). https://doi.org/10.1038/s41566-025-01716-y

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