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High-brightness all-polymer stretchable LED with charge-trapping dilution

Nature volume 603, pages 624–630 (2022)Cite this article

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Abstract

Next-generation light-emitting displays on skin should be soft, stretchable and bright1,2,3,4,5,6,7. Previously reported stretchable light-emitting devices were mostly based on inorganic nanomaterials, such as light-emitting capacitors, quantum dots or perovskites6,7,8,9,10,11. They either require high operating voltage or have limited stretchability and brightness, resolution or robustness under strain. On the other hand, intrinsically stretchable polymer materials hold the promise of good strain tolerance12,13. However, realizing high brightness remains a grand challenge for intrinsically stretchable light-emitting diodes. Here we report a material design strategy and fabrication processes to achieve stretchable all-polymer-based light-emitting diodes with high brightness (about 7,450 candela per square metre), current efficiency (about 5.3 candela per ampere) and stretchability (about 100 per cent strain). We fabricate stretchable all-polymer light-emitting diodes coloured red, green and blue, achieving both on-skin wireless powering and real-time displaying of pulse signals. This work signifies a considerable advancement towards high-performance stretchable displays.

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Fig. 1: Spontaneously formed nanofibre light-emitting structures of various colours for enhanced stretchability of light-emitting conjugated polymer films.
Fig. 2: Charge-trapping-dilution effect for enhancing electronic and optical performances of stretchable light-emitting conjugated polymer films.
Fig. 3: High-conductivity and highly stretchable PEDOT:PSS/PR electrode.
Fig. 4: Intrinsically stretchable, low-modulus and high-performance APLEDs and APLED arrays with different colours for wearable applications.

Data availability

The data that support the findings of this study are available within this article and its Supplementary Information. Additional data are available from the corresponding authors on request. Source data are provided with this paper.

Change history

  • 06 April 2022

    In the version of this article initially published, bond lines were omitted in Fig. 3a, PEDOT and PSS structures; the bonds have now been restored

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Acknowledgements

Part of this work was performed at the Stanford Nano Shared Facilities (SNSF), supported by the National Science Foundation under award ECCS-1542152. We thank Agfa-Gevaert N.V. for providing PEDOT:PSS, Daikin Co. for providing PVDF-HFP and Kaneka Co. for providing SIBS. Y.-X.W. was supported by a visiting scholar funding (201806255002) from the China Scholarship Council. N.M. was supported by a Japan Society for the Promotion of Science (JSPS) Overseas Research Fellowship. This research used resources of the Advanced Light Source, a U.S. Department of Energy Office of Science User Facility under contract no. DE-AC02-05CH11231.

Author information

Author notes

  1. These authors contributed equally: Zhitao Zhang, Weichen Wang, Yuanwen Jiang, Yi-Xuan Wang

Authors and Affiliations

  1. Department of Chemical Engineering, Stanford University, Stanford, CA, USA

    Zhitao Zhang, Weichen Wang, Yuanwen Jiang, Yi-Xuan Wang, Yilei Wu, Jian-Cheng Lai, Simiao Niu, Chengyi Xu, Chien-Chung Shih, Hongping Yan, Hung-Chin Wu, Donglai Zhong, Naoji Matsuhisa, Yu Zheng, Zhiao Yu, Jeffrey B.-H. Tok & Zhenan Bao

  2. Department of Materials Science and Engineering, Stanford University, Stanford, CA, USA

    Weichen Wang, Gan Chen, Yang Wang & Reinhold Dauskardt

  3. Tianjin Key Laboratory of Molecular Optoelectronic Sciences, Department of Chemistry, School of Science, Tianjin University, Tianjin, China

    Yi-Xuan Wang

  4. State Key Laboratory of Coordination Chemistry, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing, China

    Jian-Cheng Lai

  5. Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, CA, USA

    Cheng Wang

  6. School of Polymer Science and Engineering, University of Southern Mississippi, Hattiesburg, MS, USA

    Luke Galuska, Nathaniel Prine & Xiaodan Gu

  7. Department of Chemistry, Stanford University, Stanford, CA, USA

    Yu Zheng & Zhiao Yu

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  1. Zhitao Zhang
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Contributions

Z.Z. and Z.B. conceived the idea. Z.B. directed the project. Z.Z., W.W., Y.J. and Y.-X.W. participated in materials synthesis, device fabrication and data processing. Z.Z. and W.W. developed stretchable light-emitting materials. Z.Z., Y.J. and Y.-X.W. developed the stretchable PEDOT:PSS electrode. Y.J. performed part of the AFM, UV and PL measurements. Y.Wu performed the PLQE, lifetime and energy-level measurements. Z.Z. and J.-C.L. performed the transmittance and device modulus tests and data collections. S.N. developed the flexible wireless power supply circuit. C.X. developed the system for testing real-time pulse signals. Z.Z. and C.-C.S. developed stretchable interlayers. C.W. and H.Y. performed the R-SoXS tests. L.G. and N.P. performed the thin-film mechanics tests and part of the AFM and modulus measurements. H.-C.W. performed the GIXD tests. D.Z. helped to collect part of the optical images of the stretchable PEDOT:PSS/PR electrode. G.C. performed the XPS measurements. N.M. helped with the discussion of stretchable interlayers. Y.Z. and Z.Y. performed the dichroic ratio tests. Y.Wang performed the part of modulus measurements. Z.Z., W.W., Y.J. J.B.-H.T. and Z.B. wrote and revised the paper.

Corresponding author

Correspondence to Zhenan Bao.

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 Stanford University has filed a patent application related to this work, the patent application number is 63/314,875.

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Extended data figures and tables

Extended Data Fig. 1 AFM phase images of SY/PU films with increased PU amount.

The films were prepared by spin coating from a mixture solution of SY (7 mg ml−1) and PU (7 mg ml−1) in THF with different weight ratios and dried under vacuum (200 mTorr) for 30 min. Distinct nanofibre structures can be seen with the addition of PU.

Extended Data Fig. 2 Optical images of SY/PU films with increased PU amount at different strains.

The scale bar is 100 μm.

Extended Data Fig. 3 Photographs of stretchable light-emitting films with different colours for various wearable applications.

a, Photographs of photoluminescent images of a stretchable and patterned light-emitting polymer film under stretching and twisting. The scale bar is 5 mm. b, Photographs of photoluminescent images of a patterned light-emitting polymer film seamlessly integrated with the finger withstanding various deformations.

Extended Data Fig. 4

Spectrum of emission/absorption ratio of SY/PU films (nearly the same thickness) with increased amount of PU: collected from spin-coated films (a) and after normalization on the basis of SY unit mass (b).

Source data

Extended Data Fig. 5 2D contour plots of time-resolved PL of SY/PU films with increased PU amount while the film thicknesses were kept nearly the same.

A higher amount of PU resulted in longer lifetime, with the lifetime increasing from 1.49, 1.71, 1.72, 1.74, 1.84 to 1.85 ns.

Extended Data Fig. 6 Electron and hole current density versus driven voltage characteristics of SY/PU films with increased PU amount while the film thicknesses were kept nearly the same.

a, Electron current density–voltage curves. The trap-limited electron transport of SY/PU films with electron-only devices (ITO/Al/SY:PU/PFN-Br:PEIE/Al). The electron current densities were 0.0008, 0.0085, 0.0119, 0.0180, 0.0476 and 0.1383 A m−2, with PU amounts of 0, 30, 40, 50, 60 and 70 wt%, respectively. b, Hole current density–voltage curves. The trap-free hole transport of SY/PU films in a set of ITO/PEDOT:PSS:Triton X/SY:PU/MoO3/Au hole-only devices. The hole current densities were 52.7, 81.0, 255.4, 532.2, 327.1 and 350.7 A m−2 when increasing the PU amount.

Source data

Extended Data Fig. 7 PLED characteristics of SY/PU films on rigid ITO glass substrates with increased PU amount while the film thicknesses were kept nearly the same with the set of ITO/PEDOT:PSS:Triton X (8 nm)/TFB (40 nm)/SY:PU (120 nm)/PFN-Br:PEIE (10 nm)/Al (60 nm).

a, Current density–voltage curves. b, Luminance–voltage curves. c, Current efficiency–voltage curves. The luminance values were 10,868, 34,743, 19,227, 15,631, 11,159 and 2,365 cd m−2 with increased PU amount, whereas the current efficiencies were 4.1, 14.2, 13.1, 13.5, 13.5 and 13.3 cd A−1.

Source data

Extended Data Fig. 8 Energy level and optical bandgap for all the layers in APLEDs.

PESA measurements of SY/PU film (a), red polymer/PU film (b), green polymer/PU film (c), blue polymer/PU film (d), PFN-Br/PEIE film (e), TFB/PU film (f), PEDOT:PSS/Triton X film (g) and PEDOT:PSS/PR film (h). UV–vis absorption spectra of SY/PU film (i), red polymer/PU film (j), green polymer/PU film (k), blue polymer/PU film (l), PFN-Br/PEIE film (m) and TFB/PU film (n). Optical bandgap was estimated from the absorption edge of as-cast thin film. HOMO energies were determined by UV PESA. LUMO energies were calculated according to ELUMO = Eg + EHOMO.

Source data

Extended Data Fig. 9

Fabrication process of an intrinsically stretchable APLED.

Extended Data Fig. 10

Energy-level alignment diagrams, current density and luminance, and current efficiency–luminance curves of intrinsically stretchable APLEDs (PVDF-HFP/PEDOT:PSS:PR/PEDOT:PSS:Triton X/TFB:PU/RGB-coloured light-emitting polymers:PU/PFN-Br:PEIE/PEDOT:PSS:PR/PVDF-HFP) with red (a–c), green (d–f) and blue (g–i) colours.

Source data

Supplementary information

Supplementary Information

This file contains Supplementary Notes, Supplementary Figs. 1–30, Supplementary Tables 1–3, captions for Supplementary Videos 1–5 and Supplementary References.

Supplementary Video 1

A stretchable and multicolour light-emitting polymer film seamlessly integrated with the finger, withstanding various deformations.

Supplementary Video 2

A stretchable and multicolour light-emitting polymer film under stretching.

Supplementary Video 3

A stretchable and multicolour light-emitting polymer film under twisting.

Supplementary Video 4

A stretchable APLED seamlessly integrated with the skin under wireless powering at 9 V.

Supplementary Video 5

A stretchable APLED integrated with the skin showing real-time pulse signals.

Source data

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Zhang, Z., Wang, W., Jiang, Y. et al. High-brightness all-polymer stretchable LED with charge-trapping dilution. Nature 603, 624–630 (2022). https://doi.org/10.1038/s41586-022-04400-1

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