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Intrinsically stretchable quantum dot light-emitting diodes

Nature Electronics volume 7, pages 365–374 (2024)Cite this article

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Abstract

Stretchable displays that can change their shape and size under strain could be used to create displays with unconventional form factors. However, intrinsically stretchable light-emitting devices have poor luminous performance, such as low brightness. Here we show that intrinsically stretchable quantum dot light-emitting diodes (QLEDs) can be made using a mechanically soft and stretchable emissive layer consisting of a ternary nanocomposite of colloidal quantum dots, an elastomeric polymer and a charge transport polymer. The light-emitting layer maintains a nearly constant interparticle distance even under 50% strain, ensuring reliable operation of the QLED under stretching. The polymer-rich charge transport region at the bottom of the nanocomposite functions as a hole transport pathway to the embedded quantum dots. The QLEDs exhibit a turn-on voltage of 3.2 V and a maximum luminance of 15,170 cd m−2 at 6.2 V without loss of brightness, even when under 50% strain, and can be used to make stretchable full-colour passive-matrix QLED arrays.

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Fig. 1: Characterization of stretchable EML that consists of QDs, an elastomer and a charge transport polymer.
Fig. 2: Mechanical properties of stretchable EML.
Fig. 3: Optoelectronic properties of stretchable EML.
Fig. 4: Intrinsically stretchable QLEDs.
Fig. 5: Patterning of stretchable EML for multicolour emitting stretchable displays.

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The data that support the plots within this paper and other findings of this study are available from the corresponding authors upon reasonable request.

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The source codes for Arduino 1.8.3 are available from the corresponding authors upon reasonable request.

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Acknowledgements

This research was supported by research projects IBS-R006-D1 and IBS-R006-A1. This work was supported by the National Research Foundation of Korea (NRF) grant funded by the Korean government (MSIT) (grant nos. 2021R1C1C1007997, 2022R1A5A6000846 and 2021R1C1C1007844). This work was supported by the Samsung Research Funding & Incubation Center of Samsung Electronics under project no. SRFC-MA2002-03. We also acknowledge the support from the Institute of Engineering Research at Seoul National University. The experiments at PAL were supported in part by the MSIT, POSTECH and UNIST Central Research Facilities.

Author information

Author notes

  1. These authors contributed equally: Dong Chan Kim, Hyojin Seung, Jisu Yoo, Junhee Kim.

Authors and Affiliations

  1. Center for Nanoparticle Research, Institute for Basic Science (IBS), Seoul, Republic of Korea

    Dong Chan Kim, Hyojin Seung, Junhee Kim, Ji Su Kim, Dongjun Jung, Chansul Park, Hyeonjun Heo, Taeghwan Hyeon, Moon Kee Choi & Dae-Hyeong Kim

  2. School of Chemical and Biological Engineering, Institute of Chemical Processes, Seoul National University, Seoul, Republic of Korea

    Dong Chan Kim, Hyojin Seung, Junhee Kim, Ji Su Kim, Dongjun Jung, Chansul Park, Hyeonjun Heo, Taeghwan Hyeon & Dae-Hyeong Kim

  3. Department of Chemical and Biological Engineering, Gachon University, Seongnam, Republic of Korea

    Dong Chan Kim

  4. Department of Materials Science and Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan, Republic of Korea

    Jisu Yoo & Moon Kee Choi

  5. Department of Energy Science and Engineering, Daegu Gyeongbuk Institute of Science and Technology (DGIST), Daegu, Republic of Korea

    Hyeon Hwa Song, Kyunghoon Lee & Jiwoong Yang

  6. Graduate School of Semiconductor Materials and Devices Engineering, Center for Future Semiconductor Technology (FUST), Ulsan National Institute of Science and Technology (UNIST), Ulsan, Republic of Korea

    Yunho Kim & Moon Kee Choi

  7. Center for Opto-Electronic Materials and Devices, Post-silicon Semiconductor Institute, Korea Institute of Science and Technology (KIST), Seoul, Republic of Korea

    Changsoon Choi

  8. Department of Materials Science and Engineering, Seoul National University, Seoul, Republic of Korea

    Dae-Hyeong Kim

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Contributions

D.C.K., H.S., J. Yoo, J.K., J. Yang, M.K.C., T.H. and D.-H.K. designed the experiments, analysed the data and wrote the paper. J.K., H.H.S. and K.L. synthesized the quantum dots, made composite solutions and conducted optical analysis. D.C.K., H.S., J. Yoo, J.S.K., Y.K., C.C., D.J., C.P. and H.H. fabricated the intrinsically stretchable QLED and characterized the device performance. All authors discussed the results and commented on the manuscript.

Corresponding authors

Correspondence to Jiwoong Yang, Taeghwan Hyeon, Moon Kee Choi or Dae-Hyeong Kim.

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Nature Electronics thanks Qibing Pei, Sihong Wang and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Extended data

Extended Data Fig. 1 Characterization of binary QD-elastomer composite films.

a-f, AFM topography images and three-dimensional images (inset) of QD/SEBS-g-MA (w/w = 20:1) (a), QD/SEBS-g-MA (w/w = 10:1) (b), QD/SEBS-g-MA (w/w = 5:1) (c), QD/SBS (w/w = 10:1) (d), QD/SEBS (w/w = 10:1) (e), and bare QD (f) films. g,h, QD/SEBS-g-MA (w/w = 20:1) film under 50% of stretching. Schematic image (g) and the AFM image of the stretched film (h). i,j, QD/SEBS-g-MA (w/w = 10:1) film under 50% of stretching. Schematic image (i) and the AFM image of the stretched film. (j). k-m, Device structure of conventional QLEDs (k), J–V–L characteristics (l), and EQE data (m). In (l) and (m), three cases were compared, that is, bare QDs (black) or binary QD/SEBS-g-MA composites with different weight fractions (red for w/w = 20:1, or blue for w/w = 10:1). n, J–V characteristics of Au/EML/Au device were compared with bare QDs (black) or binary QD/SEBS-g-MA composites (red for w/w = 20:1, or blue for w/w = 10:1).

Extended Data Fig. 2 Effect of the TFB weight fraction on the size of island-shaped domains.

a, AFM topography images of binary composite films of SEBS-g-MA and TFB, with increasing TFB weight fractions. The size of island-shape domains increases as more TFB is added. b, AFM topography images of top and bottom surfaces of stretchable EML films with increasing TFB weight fractions. Similar to a, the size of island-shape domains increases as more TFB is added.

Extended Data Fig. 3 Uniaxially stretched stretchable EML films.

a, “Stretch-and-transfer” process to prepare samples of stretched films for the AFM analysis. b,c, AFM phase analysis of the stretched stretchable EML (Q100S5T5) film (b) and stretchable EML (Q100S10T5) film (c). Partial cracks are found around the TFB-rich islands in the stretchable EML (Q100S5T5) film, while the embossed structure is formed in the stretchable EML (Q100S10T5) film.

Extended Data Fig. 4 The inter-particle distance of the stretchable EML (Q100S10T5) film.

a, Raw data of GISAXS measured with the films under strains of 0, 10, 30, and 50%. b,c, GISAXS analysis in the in-plane (b) and out-of-plane direction (c). d, Schematic illustrations of the stretchable EML film with the same volume and interplanar distances (for example, dxy, dz) before (left) and after (right) the stretching.

Extended Data Fig. 5 Photoluminescence properties and exciton quenching of the stretchable EML.

a,b, Photoluminescence (PL) properties of the stretchable EML solution with different TFB weight fractions under 480 nm excitation. Steady-state (a) and time-resolved PL (b). c, Time-resolved PL of the Q100S10T5 film and Q100T5 film. d-f, Morphology of the QD/TFB binary blend film. Schematic illustration (d), AFM image (e), and cross-sectional TEM image (f) of the Q100T5 film, exhibiting the distributed QD-TFB interface inside the blended film.

Extended Data Fig. 6 Fabrication and characterization of intrinsically stretchable QLEDs.

a, Illustrations show the step-by-step fabrication process of the intrinsically stretchable QLEDs. b, Stretchability of the PEDOT:PSS/FS-31 composite film. c, d, Optical (c) and AFM images (d) of the double-layered structure of the TFB/stretchable EML film, stretched under 60% applied strain. The inset schematic image in panel (c) shows the structure of double-layered films. e, Optical images of the pristine ZnO film (upper panel) and the ZnO/PFN-Br composite film (lower panel) stretched under 20% applied strain. f, AFM images of the double-layered structure of the pristine ZnO/stretchable EML film (upper panel), and the ZnO/PFN-Br/stretchable EML film (lower panel) stretched under 60% applied strain. g, Resistance increase of stretchable anodes and cathodes under the applied strain. h, EQE of the intrinsically stretchable QLED under increasing voltage. i, Device lifetime of the intrinsically stretchable QLED. j, Cyclic stretching test data of the intrinsically stretchable QLED.

Extended Data Fig. 7 Green-emitting intrinsically stretchable QLED and PM-QLED array.

a-d, Intrinsically stretchable QLEDs under various deformation states. The devices exhibit outstanding mechanical stability under 1-D stretching (a, b), twisting (c), and crumpling (d). e, Snapshots of Supplementary Movie 1. Scan speed adjustment of intrinsically stretchable PM-QLED array, operated under common cathode configuration. Scan speed should be faster than 1 ms per line to display a pattern without flickering.

Extended Data Fig. 8 A customized circuit for the operation of the intrinsically stretchable PM-QLED arrays.

a, Circuit diagram of the experimental setup for the operation of the PM-QLED array. The MCU board (teensy 3.6), 16 channel DAC (AD5767), and voltage reference (ADR4525BRZ) were used in the setup. b, Photograph of the experimental setup.

Extended Data Fig. 9 Aligned multiple transfer printing of the intrinsically stretchable EML patterns.

a, Device performance of QLEDs using red-emitting stretchable EMLs. b, Device performance of QLEDs using blue-emitting stretchable EMLs. c, d, Transfer printing of rectangular patterns of stretchable EML with various pattern sizes (c). The highest resolution of transfer printing is ~100 μm (d). e-h, Aligned transfer printing of RGB stretchable EML patterns. Red (e), green (f), blue (g), and red/green (h) stretchable EML patterns are printed in an aligned manner on the stretchable substrate. i-k, PL images of the printed stretchable EML patterns. Original images (i), 1D-stretched image under 50% uniaxial strain (j), and 2D-stretched image under 50% biaxial strain (k).

Extended Data Table 1 Performance of reported intrinsically stretchable light-emitting devices
Full size table

Supplementary information

Supplementary Video 1

Operation of the intrinsically stretchable PM-QLED arrays.

Supplementary Video 2

Operation of the multicolour intrinsically stretchable QLEDs.

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Kim, D.C., Seung, H., Yoo, J. et al. Intrinsically stretchable quantum dot light-emitting diodes. Nat Electron 7, 365–374 (2024). https://doi.org/10.1038/s41928-024-01152-w

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