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Patterning organic single-crystal transistor arrays

Abstract

Field-effect transistors made of organic single crystals are ideal for studying the charge transport characteristics of organic semiconductor materials1. Their outstanding device performance2,3,4,5,6,7,8, relative to that of transistors made of organic thin films, makes them also attractive candidates for electronic applications such as active matrix displays and sensor arrays. These applications require minimal cross-talk between neighbouring devices. In the case of thin film systems, simple patterning of the active semiconductor layer9,10 minimizes cross-talk. But when using organic single crystals, the only approach currently available for creating arrays of separate devices is manual selection and placing of individual crystals—a process prohibitive for producing devices at high density and with reasonable throughput. In contrast, inorganic crystals have been grown in extended arrays11,12,13, and efficient and large-area fabrication of silicon crystalline islands with high mobilities for electronic applications has been reported14,15. Here we describe a method for effectively fabricating large arrays of single crystals of a wide range of organic semiconductor materials directly onto transistor source–drain electrodes. We find that film domains of octadecyltriethoxysilane microcontact-printed onto either clean Si/SiO2 surfaces or flexible plastic provide control over the nucleation of vapour-grown organic single crystals. This allows us to fabricate large arrays of high-performance organic single-crystal field-effect transistors with mobilities as high as 2.4 cm2 V-1 s-1 and on/off ratios greater than 107, and devices on flexible substrates that retain their performance after significant bending. These results suggest that our fabrication approach constitutes a promising step that might ultimately allow us to utilize high-performance organic single-crystal field-effect transistors for large-area electronics applications.

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Figure 1: Patterning of organic single crystals.
Figure 2: Controlling pentacene crystal nucleation.
Figure 3: Single-crystal transistor arrays on rigid substrates.
Figure 4: Flexible single-crystal transistor arrays.

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References

  1. de Boer, R. W. I., Gershenson, M. E., Morpurgo, A. F. & Podzorov, V. Organic single-crystal field-effect transistors. Phys. Status Solidi a 201, 1302–1331 (2004)

    Article  ADS  CAS  Google Scholar 

  2. Briseno, A. L. et al. Patterned growth of large oriented organic semiconductor single crystals on self-assembled monolayer templates. J. Am. Chem. Soc. 127, 12164–12165 (2005)

    Article  CAS  PubMed  Google Scholar 

  3. Huitema, H. E. A. et al. Plastic transistors in active-matrix displays. Nature 414, 599 (2001)

    Article  ADS  CAS  PubMed  Google Scholar 

  4. Moon, H. et al. Synthesis, crystal structure, and transistor performance of tetracene derivatives. J. Am. Chem. Soc. 126, 15322–15323 (2004)

    Article  CAS  PubMed  Google Scholar 

  5. Podzorov, V. et al. Intrinsic charge transport on the surface of organic semiconductors. Phys. Rev. Lett. 93, 086602 (2004)

    Article  ADS  CAS  PubMed  Google Scholar 

  6. Pope, M., Charles, E. & Swenberg, C. E. Electronic Processes in Organic Crystals and Polymers (Oxford Univ. Press, New York, 1999)

    Google Scholar 

  7. Sundar, V. C. et al. Elastomeric transistor stamps: Reversible probing of charge transport in organic crystals. Science 303, 1644–1646 (2004)

    Article  ADS  CAS  PubMed  Google Scholar 

  8. Zeis, R. et al. Field effect studies on rubrene and impurities of rubrene. Chem. Mater. 18, 244–248 (2006)

    Article  CAS  Google Scholar 

  9. Steudel, S., Janssen, D., Verlaak, S., Genoe, J. & Heremans, P. Patterned growth of pentacene. Appl. Phys. Lett. 85, 5550–5552 (2004)

    Article  ADS  CAS  Google Scholar 

  10. De Vusser, S., Steudel, S., Myny, K., Genoe, J. & Heremans, P. Integrated shadow mask method for patterning small molecule organic semiconductors. Appl. Phys. Lett. 88, 103501 (2006)

    Article  ADS  Google Scholar 

  11. Aizenberg, J., Black, A. J. & Whitesides, G. M. Controlling local disorder in self-assembled monolayers by patterning the topography of their metallic supports. Nature 394, 868–871 (1998)

    Article  ADS  CAS  Google Scholar 

  12. Aizenberg, J., Black, A. J. & Whitesides, G. M. Control of crystal nucleation by patterned self-assembled monolayers. Nature 398, 495–498 (1999)

    Article  ADS  CAS  Google Scholar 

  13. He, J. H. et al. Pattern and feature designed growth of ZnO nanowire arrays for vertical devices. J. Phys. Chem. B 110, 50–53 (2006)

    Article  CAS  PubMed  Google Scholar 

  14. van der Wilt, P. C., van Dijk, B. D., Bertens, G. J., Ishihara, R. & Beenakker, C. I. M. Formation of location-controlled crystalline islands using substrate-embedded seeds in excimer-laser crystallization of silicon films. Appl. Phys. Lett. 79, 1819–1821 (2001)

    Article  ADS  CAS  Google Scholar 

  15. Vikas, R. et al. in Proc. International Electron Devices Meeting 2005 919–922. (IEEE International, 2005)

  16. Kloc, C., Simpkins, P. G., Siegrist, T. & Laudise, R. A. Physical vapor growth of centimeter-sized crystals of alpha-hexathiophene. J. Cryst. Growth 182, 416–427 (1997)

    Article  ADS  CAS  Google Scholar 

  17. Choi, H. Y., Kim, S. H. & Jang, J. Self-organized organic thin-film transistors on plastic. Adv. Mater. 16, 732–736 (2004)

    Article  CAS  Google Scholar 

  18. Ruiz, R. et al. Pentacene thin film growth. Chem. Mater. 16, 4497–4508 (2004)

    Article  CAS  Google Scholar 

  19. Heringdorf, F., Reuter, M. C. & Tromp, R. M. Growth dynamics of pentacene thin films. Nature 412, 517–520 (2001)

    Article  ADS  Google Scholar 

  20. Markov, I. V. Crystal Growth for Beginners (World Scientific, Singapore, 2003)

    Book  Google Scholar 

  21. Venables, J. A., Spiller, G. D. T. & Hanbucken, M. Nucleation and growth of thin films. Rep. Prog. Phys. 47, 399–459 (1984)

    Article  ADS  Google Scholar 

  22. Granasy, L., Borzsonyi, T. & Pusztai, T. Nucleation and bulk crystallization in binary phase field theory. Phys. Rev. Lett. 88, 206105 (2002)

    Article  ADS  PubMed  Google Scholar 

  23. Granasy, L. et al. Phase field theory of crystal nucleation and polycrystalline growth: A review. J. Mater. Res. 21, 309–319 (2006)

    Article  ADS  CAS  Google Scholar 

  24. Verlaak, S., Steudel, S., Heremans, P., Janssen, D. & Deleuze, M. S. Nucleation of organic semiconductors on inert substrates. Phys. Rev. B 68, 195409 (2003)

    Article  ADS  Google Scholar 

  25. Kelley, T. W. et al. Recent progress in organic electronics: Materials, devices, and processes. Chem. Mater. 16, 4413–4422 (2004)

    Article  CAS  Google Scholar 

  26. Klauk, H., Gundlach, D. J., Nichols, J. A. & Jackson, T. N. Pentacene organic thin-film transistors for circuit and display applications. IEEE Trans. Electron Devices 46, 1258–1263 (1999)

    Article  ADS  CAS  Google Scholar 

  27. Klauk, H. et al. High-mobility polymer gate dielectric pentacene thin film transistors. J. Appl. Phys. 92, 5259–5263 (2002)

    Article  ADS  CAS  Google Scholar 

  28. Briseno, A. L. et al. High-performance organic single-crystal transistors on flexible substrates. Adv. Mater. 18, 2320–2324 (2006)

    Article  CAS  Google Scholar 

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Acknowledgements

A.L.B. acknowledges a Bell Labs Graduate Research Fellowship. A.L.B., F.W., R.J.T. and Y.Y. acknowledge financial support from the Air Force Office of Scientific Research (AFOSR). S.C.B.M. acknowledges financial support from the Deutsche Forschungsgemeinschaft, and Z.B. acknowledges partial support from the Stanford Center for Polymeric Interfaces and Macromolecular Assemblies (NSF-Center MRSEC), the Stanford School of Engineering, and a Sloan Research Fellowship. Author Contributions A.L.B. performed single-crystal patterning on substrates and FET devices, measurements on FET devices, and wrote most of the manuscript. S.C.B.M. elucidated the growth mechanism, performed AFM measurements, and wrote parts of the manuscript. M.M.L. assisted in sample preparation and assisted in device measurements and calculations. S.L. assisted in crystal patterning, device preparation, and performed SEM measurements. R.J.T. assisted in flexible device preparation, measurements and calculations. C.R. designed and fabricated the transistor array devices and PDMS stamp masters via lithography. M.E.R. assisted in early experiments and purified some of the organic source materials. Y.Y. provided use of laboratory space and instruments. F.W. provided feedback and suggestions on experiments. Z.B. conceptualized and directed the research project. All authors discussed the results and commented on the manuscript.

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Correspondence to Zhenan Bao.

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Supplementary Notes

This file contains Supplementary Notes with a more detailed description of the method, additional experimental data on the organic single crystals morphology and corresponding transistor performance, and supporting evidence for the proposed nucleation mechanism, including 20 new Supplementary Figures some of which are referenced from within the main text . (PDF 6243 kb)

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Briseno, A., Mannsfeld, S., Ling, M. et al. Patterning organic single-crystal transistor arrays. Nature 444, 913–917 (2006). https://doi.org/10.1038/nature05427

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