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Monolithically integrated high-density vertical organic electrochemical transistor arrays and complementary circuits

Nature Electronics volume 7, pages 234–243 (2024)Cite this article

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Abstract

Organic electrochemical transistors (OECTs) can be used to create biosensors, wearable devices and neuromorphic systems. However, restrictions in the micro- and nanopatterning of organic semiconductors, as well as topological irregularities, often limit their use in monolithically integrated circuits. Here we show that the micropatterning of organic semiconductors by electron-beam exposure can be used to create high-density (up to around 7.2 million OECTs per cm2) and mechanically flexible vertical OECT arrays and circuits. The energetic electrons convert the semiconductor exposed area to an electronic insulator while retaining ionic conductivity and topological continuity with the redox-active unexposed areas essential for monolithic integration. The resulting p- and n-type vertical OECT active-matrix arrays exhibit transconductances of 0.08–1.7 S, transient times of less than 100 μs and stable switching properties of more than 100,000 cycles. We also fabricate vertically stacked complementary logic circuits, including NOT, NAND and NOR gates.

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Fig. 1: Fabrication and monolithic integration of vOECTs using e-beam patterning.
Fig. 2: vOECT ionic and electronic transport characterization and transient response stability.
Fig. 3: Characterization of e-beam unexposed and exposed OSC films.
Fig. 4: High-density monolithically integrated vOECT arrays fabricated by e-beam exposure.
Fig. 5: 2D areal mapping and flexible vOECT arrays.
Fig. 6: High-resolution vertically stacked complementary circuits.

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Source data are provided with this paper. Additional data related to this work are available from the corresponding authors upon request.

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Acknowledgements

This work was supported by the AFOSR (contract no. FA9550-22-1-0423), the US Office of Naval Research Contract no. N00014-20-1-2116, by the US Department of Commerce, National Institute of Standards and Technology as part of the Centre for Hierarchical Materials Design Award no. 70NANB10H005, BSF (award no. 2020384), NSF (DMR-2223922) and the Northwestern University Materials Research Science and Engineering Center Awards NSF DMR-1720139 and DMR-2308691. J.R. gratefully acknowledges support from the Alfred P. Sloan Foundation (FG-2019-12046). This work acknowledges the US Department of Energy under contract no. DE-AC02-05CH11231 at beamline 8-ID-E of the Advanced Photon Source, a US Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. This work made use of the NUFAB facility of Northwestern University’s NUANCE Center, which has received support from the SHyNE Resource (NSF ECCS-2025633), the IIN and Northwestern’s MRSEC programme (NSF DMR-1720139).

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Authors and Affiliations

  1. Department of Chemistry and Materials Research Center, Northwestern University, Evanston, IL, USA

    Jaehyun Kim, Robert M. Pankow, Yongjoon Cho, Isaiah D. Duplessis, Fei Qin, Ding Zheng, Wei Huang, Tobin J. Marks & Antonio Facchetti

  2. Department of Semiconductor Science, Dongguk University, Seoul, Republic of Korea

    Jaehyun Kim

  3. Department of Materials Science and Engineering, Northwestern University, Evanston, IL, USA

    Dilara Meli, Jonathan Rivnay & Tobin J. Marks

  4. Department of Biomedical Engineering, Northwestern University, Evanston, IL, USA

    Rachel Daso & Jonathan Rivnay

  5. Laboratory of Organic Electronics, Department of Science and Technology, Linköping University, SE-601 74, Norrköping, Sweden

    Antonio Facchetti

  6. School of Materials Science and Engineering, Georgia Institute of Technology, Atlanta, GA, USA

    Antonio Facchetti

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Contributions

J.K., T.J.M. and A.F. conceived and designed the research. J.K. carried out the device fabrication, characterizations and demonstrations. R.M.P. and Y.C. synthesized the polymer semiconductors. J.K., R.M.P., I.D.D., F.Q., D.Z. and W.H. analysed the data. D.M., R.D. and J.R. conducted the bandwidth and EIS measurements. R.M.P. and I.D.D. measured and analysed the GIWAXS. All the authors discussed the results and commented on the manuscript. J.K., J.R., T.J.M. and A.F. wrote the manuscript.

Corresponding authors

Correspondence to Jonathan Rivnay, Tobin J. Marks or Antonio Facchetti.

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A patent application has been filed by Northwestern with inventors J.K., T.J.M. and A.F. The remaining authors declare no competing interests.

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Nature Electronics thanks Wei Lin Leong and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Kim, J., Pankow, R.M., Cho, Y. et al. Monolithically integrated high-density vertical organic electrochemical transistor arrays and complementary circuits. Nat Electron 7, 234–243 (2024). https://doi.org/10.1038/s41928-024-01127-x

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