Abstract
Advanced transfer printing technologies have enabled the fabrication of high-performance flexible and stretchable devices, revolutionizing many research fields including soft electronics, optoelectronics, bioelectronics and energy devices. Despite previous innovations, challenges remain, such as safety concerns due to toxic chemicals, the expensive equipment, film damage during the transfer process and difficulty in high-temperature processing. Thus a new transfer printing process is needed for the commercialization of high-performance soft electronic devices. Here we propose a damage-free dry transfer printing strategy based on stress control of the deposited thin films. First, stress-controlled metal bilayer films are deposited using direct current magnetron sputtering. Subsequently, mechanical bending is applied to facilitate the release of the metal bilayer by increasing the overall stress. Experimental and simulation studies elucidate the stress evolution mechanisms during the processes. By using this method, we successfully transfer metal thin films and high-temperature-treated oxide thin films onto flexible or stretchable substrates, enabling the fabrication of two-dimensional flexible electronic devices and three-dimensional multifunctional devices.
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Data availability
The data that support the other findings of this study are available from the corresponding authors upon reasonable request. Source data are provided with this paper.
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Acknowledgements
We acknowledge the following funding sources: Institute for Basic Science, Republic of Korea, (no. IBS-R006-A1; Y.S., S.H., C.L., K.D., D.-H.K. and S.L.) and the National Research Foundation of Korea (NRF) grant funded by the Korean government (Ministry of Science, ICT and Future Planning, MSIP; no. 2021M3H4A6A01045764; J.H.K.).
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Y.S., S.H., C.L. and S.L. designed the experiments. Y.S., S.H., C.L. and S.L. performed the experiments and analysis. Y.S. performed analytical modelling. Y.C.H. and J.H.K. designed and performed the stress modelling. S.H., K.D. and S.L. performed TFB-related experiments. Y.S., S.H., Y.C.H., J.H.K., D.-H.K. and S.L. drafted the manuscript. S.L., D.-H.K. and J.H.K. are corresponding authors of this work.
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Extended data
Extended Data Fig. 1 Characteristics of dry transfer method using stress engineering.
a, Generation of stress and its gradient by bilayer formation and mechanical bending. b, Easy peeling mechanism of bilayer formation and bending deformation. c, Transfer of a thin film subjected to high-temperature oxidation process without forming interfacial diffusion between the device and the substrate.
Extended Data Fig. 2 Examples of tensile stress formation that inspires the development of the damage-free transfer printing.
a, Tensile stress evolution during thin film deposition: Formation of columnar structure (left), and residual stress generation (right): i) recrystallization model and ii) grain boundary model. b, Stress-gradient generation by forming a bilayer with two different lattice constants, c, Mechanical tensile stress created by bending deformation.
Extended Data Fig. 3 Analytical model of the single layer, bilayer and mechanical bending deformation.
a, Idealized representation of the stress distribution across the single layer film and substrate. b, An analytical method for the stress distribution in bilayer structure. c, Modeling of the cantilever deflection: (i) Stress distribution of the bilayer film, (ii) Determining the average stress of the film through force balance, (iii) Determining the bending moment of the film that as detached from the substrate, (iv) Calculation of the deflection of the film. d, Simulated result of the cantilever deflection in bilayer films. e, An analytical method for the stress distribution under outward bending.
Extended Data Fig. 4 Analysis of strain release rate of thin film.
a, The residual stress profile divided into two components: average stress and gradient. b, Strain energy release rate divided into two components: in-plane strain energy release rate and bending strain energy release rate. c, Variation in the stress and energy release rate depending on the bending height of the wafer (residual stress = 800 MPa). d, Variation in energy release rate before and after bending under different residual stresses (bending height: 2.5 mm).
Extended Data Fig. 5 Limitations of weak adhesion metals such as Ni, Cu, and Mo as a current collector for LiCoO2 cathode material.
a–c, Pictures of LCO on Pt (a), Ni (b), and Cu (c) annealed at the crystallization conditions (700 °C for 30 min, in oxygen or ambient atmosphere). d–f, XRD patterns of LCO on Pt (d), Ni (e), and Cu (f) before and after annealing. Lower patterns correspond to the pre-crystallized samples of LCO thin films.
Extended Data Fig. 6 Measurement of surface profile of Pt/LiCoO2 on Si/SiO2 wafer.
a, Surface profile of Pt thin film on Si/SiO2 wafer. b, Surface profile variation when LiCoO2 thin film is deposited. c, Surface profile of the sample after annealing at 700 °C for 30 min, in oxygen or ambient atmosphere. The profiles were measured with specimens 6 cm long and 1 cm wide.
Supplementary information
Supplementary Information
Supplementary Notes 1–11, Tables 1 and 2, Figs. 1–7 and captions for Videos 1–3.
Supplementary Video 1
Retrieval of the patterned Pt bilayer thin film onto the PDMS stamp.
Supplementary Video 2
Delamination of the deposited Pt thin film when tensile stress is generated inside the film.
Supplementary Video 3
Delamination of the Pt bilayer thin film.
Supplementary Data 1
The sin2ψ versus d-spacing data.
Supplementary Data 2
Adhesion force.
Supplementary Data 3
Voltage profile of the TFB.
Source data
Source Data Fig. 1
Stress distribution analysis through numerical simulations.
Source Data Fig. 2
Residual stress data, sin2ψ versus d-spacing data and interfacial fracture toughness versus strain energy release rates.
Source Data Fig. 4
Calibration curves and continuous monitoring of fluid.
Source Data Fig. 5
Voltage profile and cycle performance of TFB.
Source Data Extended Data Fig. 3
Simulation data.
Source Data Extended Data Fig. 4
Stress and energy release rate.
Source Data Extended Data Fig. 5
XRD patterns.
Source Data Extended Data Fig. 6
Surface profiles.
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Shin, Y., Hong, S., Hur, Y.C. et al. Damage-free dry transfer method using stress engineering for high-performance flexible two- and three-dimensional electronics. Nat. Mater. (2024). https://doi.org/10.1038/s41563-024-01931-y
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DOI: https://doi.org/10.1038/s41563-024-01931-y
