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Multi-scale ordering in highly stretchable polymer semiconducting films


Stretchable semiconducting polymers have been developed as a key component to enable skin-like wearable electronics, but their electrical performance must be improved to enable more advanced functionalities. Here, we report a solution processing approach that can achieve multi-scale ordering and alignment of conjugated polymers in stretchable semiconductors to substantially improve their charge carrier mobility. Using solution shearing with a patterned microtrench coating blade, macroscale alignment of conjugated-polymer nanostructures was achieved along the charge transport direction. In conjunction, the nanoscale spatial confinement aligns chain conformation and promotes short-range π–π ordering, substantially reducing the energetic barrier for charge carrier transport. As a result, the mobilities of stretchable conjugated-polymer films have been enhanced up to threefold and maintained under a strain up to 100%. This method may also serve as the basis for large-area manufacturing of stretchable semiconducting films, as demonstrated by the roll-to-roll coating of metre-scale films.

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The authors declare that all data supporting the findings of this study are available within the paper and its Supplementary Information. Other supporting data are available from the corresponding author upon request.

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This work is supported by the US Department of Energy, Office of Science, Basic Energy Sciences, under award DE-SC0016523 (material characterization) and by Samsung Electronics (device fabrication and characterization). G.-J.N.W. was supported by the Air Force Office of Scientific Research (grant no. FA9550-18-1-0143). Y.-H.K. acknowledges support from the NRF Korea (2018R1A2A105078734). L.S. acknowledges support from the Kodak Graduate Fellowship. The GIXD measurements were made at beamlines 11-3 and 7-2 of the Stanford Synchrotron Radiation Light Source, which are supported by the Director, Office of Science, Office of Basic Energy Sciences, of the US Department of Energy. Part of this work was performed at the Stanford Nano Shared Facilities (SNSF), supported by the National Science Foundation under award ECCS-1542152.

Author information

J.X. and Z.B. conceived and designed the experiments; J.X., H.-C.W., A.E. and K.G. fabricated the films; J.X., H.-C.W., C.Z., A.E. and M.N. fabricated the transistor devices and made the measurements; J.X. and L.S. carried out the flow simulations; X.G., F.M.-L. and H.-C.W. did the GIXD characterizations; S.C. and V.R.F. carried out the XPS and SEM characterizations; S.W., Y.K. and Y.-Q.Z. fabricated the micro-structured blades; G.-J.N.W., T.K., Y.-H.K., and H.Y. provided the conjugated polymers; S.L., D.Z. and J.L. contributed to the initial design of the printing ink. J.W.C. and B.M. advised on the discussion of results. J.X. organized the data and wrote the first draft of the manuscript. All authors reviewed and commented on the manuscript. Z.B. directed the project.

Competing interests

The authors declare no competing interests.

Correspondence to Zhenan Bao.

Supplementary information

Supplementary Information

Supplementary Figs. 1–29, Supplementary Tables 1–6, Supplementary Video Legend 1, Supplementary References

Supplementary Video 1

Roll-to-roll coating of a large-area stretchable semiconducting film.

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Fig. 1: Achieving multiple length scale ordering of conjugated polymers in stretchable semiconductors through a combination of the patterned-blade solution-shearing method and the nanoconfinement effect.
Fig. 2: Characterization of the electrical performance of the semiconducting films fabricated using different processes.
Fig. 3: Measurements of bandgap energies and activation energies for charge transport.
Fig. 4: Fully stretchable transistors fabricated from the SS-CONPHINE film.
Fig. 5: Large-area roll-to-roll coating of aligned, stretchable CONPHINE film.