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Two-dimensional charge transport in self-organized, high-mobility conjugated polymers

Nature volume 401, pages 685–688 (1999)Cite this article

Abstract

Self-organization in many solution-processed, semiconducting conjugated polymers results in complex microstructures, in which ordered microcrystalline domains are embedded in an amorphous matrix1. This has important consequences for electrical properties of these materials: charge transport is usually limited by the most difficult hopping processes and is therefore dominated by the disordered matrix, resulting in low charge-carrier mobilities2 (⩽10-5 cm2 V-1 s-1). Here we use thin-film, field-effect transistor structures to probe the transport properties of the ordered microcrystalline domains in the conjugated polymer poly(3-hexylthiophene), P3HT. Self-organization in P3HT results in a lamella structure with two-dimensional conjugated sheets formed by interchain stacking. We find that, depending on processing conditions, the lamellae can adopt two different orientations—parallel and normal to the substrate—the mobilities of which differ by more than a factor of 100, and can reach values as high as 0.1 cm2 V-1 s-1 (refs 3, 4). Optical spectroscopy of the field-induced charge, combined with the mobility anisotropy, reveals the two-dimensional interchain character of the polaronic charge carriers, which exhibit lower relaxation energies than the corresponding radical cations on isolated one-dimensional chains. The possibility of achieving high mobilities via two-dimensional transport in self-organized conjugated lamellae is important for applications of polymer transistors in logic circuits5 and active-matrix displays4,6.

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Figure 1: Two different orientations of ordered P3HT domains with respect to the FET substrate.
Figure 2: Charge carrier mobility of P3HT field-effect transistors with different microstructures.
Figure 3: Charge modulation spectroscopy of semitransparent P3HT FETs in the accumulation regime.

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Acknowledgements

We thank J. Cornil, D. Dos Santos, and A. J. Flewitt for contributions. Financial support from the European Commission and the Training and Mobility of Researchers (TMR) programme is acknowledged. H.S. thanks the Royal Society for a University Research Fellowship.

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Authors and Affiliations

  1. Cavendish Laboratory, University of Cambridge, Madingley Road, Cambridge, CB3 0HE, UK

    H. Sirringhaus, P. J. Brown & R. H. Friend

  2. Condensed Matter Physics and Chemistry Department, Risø National Laboratory, Roskilde, 4000, Denmark

    M. M. Nielsen & K. Bechgaard

  3. Laboratory of Macromolecular and Organic Chemistry, Eindhoven University of Technology, Eindhoven, 5600 MB, The Netherlands

    B. M. W. Langeveld-Voss, A. J. H. Spiering, R. A. J. Janssen & E. W. Meijer

  4. Philips Research Laboratories, Prof. Holstlaan 4, Eindhoven, 5656 AA, The Netherlands

    P. Herwig & D. M. de Leeuw

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  1. H. Sirringhaus
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  2. P. J. Brown
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  11. D. M. de Leeuw
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Correspondence to H. Sirringhaus.

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Sirringhaus, H., Brown, P., Friend, R. et al. Two-dimensional charge transport in self-organized, high-mobility conjugated polymers. Nature 401, 685–688 (1999). https://doi.org/10.1038/44359

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