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Transiently delocalized states enhance hole mobility in organic molecular semiconductors

Nature Materials volume 22, pages 1361–1369 (2023)Cite this article

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Abstract

Evidence shows that charge carriers in organic semiconductors self-localize because of dynamic disorder. Nevertheless, some organic semiconductors feature reduced mobility at increasing temperature, a hallmark for delocalized band transport. Here we present the temperature-dependent mobility in two record-mobility organic semiconductors: dinaphtho[2,3-b:2′,3′-f]thieno[3,2-b]-thiophene (DNTT) and its alkylated derivative, C8-DNTT-C8. By combining terahertz photoconductivity measurements with atomistic non-adiabatic molecular dynamics simulations, we show that while both crystals display a power-law decrease of the mobility (μ) with temperature (T) following μ ∝ T −n, the exponent n differs substantially. Modelling reveals that the differences between the two chemically similar semiconductors can be traced to the delocalization of the different states that are thermally accessible by charge carriers, which in turn depends on their specific electronic band structure. The emerging picture is that of holes surfing on a dynamic manifold of vibrationally dressed extended states with a temperature-dependent mobility that provides a sensitive fingerprint for the underlying density of states.

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Fig. 1: Molecular herringbone layer packing for the investigated OSs.
Fig. 2: T-dependent photoconductivity studies by OPTP spectroscopy in DNTT and C8-DNTT-C8.
Fig. 3: Frequency-dependent THz photoconductivity.
Fig. 4: DOS and state-resolved IPR.
Fig. 5: Temperature-dependent IPR and experimental and theoretical charge mobilities for DNTT and C8-DNTT-C8.

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Data availability

The datasets generated and/or analysed during the current study are available in the Zenodo repository, https://zenodo.org/record/8109807. The full data for this study total a couple of terabytes and are in cold storage accessible by the corresponding authors and available upon reasonable request.

Code availability

The custom FOB-SH code for non-adiabatic molecular dynamics, the python code used for the DA analysis and other post-processing tools used for this study are available from the corresponding authors upon request.

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Acknowledgements

S.G. and M. Bardini acknowledge C. Quarti for useful discussions. We are grateful to H. Burg and R. Berger for conducting scanning force microscopy measurements. This work received funding from the European Union’s Horizon 2020 research and innovation programme under Marie Sklodowska-Curie grant no. 811284. J.H., K.B. and F.S. acknowledge funding by the German Research Foundation (BR4869/4-1 and SCHR 700/40-1). G.S. acknowledges financial support from the Francqui Foundation (Francqui Start-Up Grant) and the Belgian National Fund for Scientific Research (FNRS) for financial support through research project COHERENCE2 (N°F.4536.23). Y.H.G. is thankful to the FNRS for financial support through research projects Pi-Fast (no. T.0072.18) and Pi-Chir (no. T.0094.22). J.J.G. gratefully acknowledges support from the Alexander von Humboldt Foundation. The work in Mons has been funded by the Fund for Scientific Research (FRS) of FNRS within the Consortium des Équipements de Calcul Intensif (CÉCI) under grant 2.5020.11, and by the Walloon Region (ZENOBE Tier-1 supercomputer) under grant 1117545. G.S. is a FNRS Research Associate. D.B. is a FNRS research director.

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  1. These authors contributed equally: Samuele Giannini, Lucia Di Virgilio.

Authors and Affiliations

  1. Laboratory for Chemistry of Novel Materials, University of Mons, Mons, Belgium

    Samuele Giannini, Marco Bardini & David Beljonne

  2. Max Planck Institute for Polymer Research, Mainz, Germany

    Lucia Di Virgilio, Jaco J. Geuchies, Wenhao Zheng, Hai I. Wang & Mischa Bonn

  3. Institut für Angewandte Physik, Universität Tübingen, Tübingen, Germany

    Julian Hausch, Katharina Broch & Frank Schreiber

  4. Laboratoire de Chimie des Polymères, Faculté des Sciences, Université Libre de Bruxelles (ULB), Bruxelles, Belgium

    Martina Volpi, Yves H. Geerts & Guillaume Schweicher

  5. Department of Physics and Astronomy and Thomas Young Centre, University College London, London, UK

    Jan Elsner & Jochen Blumberger

  6. International Solvay Institutes for Physics and Chemistry, Université Libre de Bruxelles (ULB), Bruxelles, Belgium

    Yves H. Geerts

  7. Nanophotonics, Debye Institute for Nanomaterials Science, Utrecht University, Utrecht, The Netherlands

    Hai I. Wang

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Contributions

S.G. performed most of the quantum chemical calculations presented in this work and performed related data analysis (with input from J.E. and M. Bardini). M. Bardini and S.G. ran non-adiabatic dynamics simulations of charge transport for the systems investigated in this work. L.D.V. conducted the THz spectroscopy experiments and analysed the data together with M. Bardini. J.J.G., J.H. and K.B. prepared samples. L.D.V. and S.G. also performed the analysis of the experimental data using the DA model. M.V. synthesized C8-DNTT-C8. G.S. contributed to sample preparation and data interpretation. J.J.G. performed X-ray diffraction measurements. M. Bonn and Y.H.G. initiated the experimental study of charge transport in thienoacene semiconductors, at short length scales and timescales. D.B., J.B., H.I.W., F.S. and M. Bonn contributed to the data interpretation, and D.B., H.I.W. and M. Bonn supervised all aspects of the research. S.G., L.D.V., H.I.W. and D.B. designed the research and wrote the manuscript. All authors reviewed and discussed the manuscript.

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Correspondence to Samuele Giannini, Hai I. Wang, Mischa Bonn or David Beljonne.

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Giannini, S., Di Virgilio, L., Bardini, M. et al. Transiently delocalized states enhance hole mobility in organic molecular semiconductors. Nat. Mater. 22, 1361–1369 (2023). https://doi.org/10.1038/s41563-023-01664-4

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