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Conductivity in organic semiconductors hybridized with the vacuum field

Abstract

Much effort over the past decades has been focused on improving carrier mobility in organic thin-film transistors by optimizing the organization of the material or the device architecture. Here we take a different path to solving this problem, by injecting carriers into states that are hybridized to the vacuum electromagnetic field. To test this idea, organic semiconductors were strongly coupled to plasmonic modes to form coherent states that can extend over as many as 105 molecules and should thereby favour conductivity. Experiments show that indeed the current does increase by an order of magnitude at resonance in the coupled state, reflecting mostly a change in field-effect mobility. A theoretical quantum model confirms the delocalization of the wavefunctions of the hybridized states and its effect on the conductivity. Our findings illustrate the potential of engineering the vacuum electromagnetic environment to modify and to improve properties of materials.

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Figure 1: Light–matter strong coupling with organic semiconductors.
Figure 2: Conductivity measurements under strong coupling on Ag and Al arrays.
Figure 3: Conductivity under strong coupling on Al arrays and gating.
Figure 4: Theoretical model.

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Acknowledgements

This work was supported in part by USIAS, the ERC through the projects Plasmonics (227557), Suprafunction (257305), and Coldsim (307688), the International Center for Frontier Research in Chemistry (icFRC, Strasbourg), the ANR Equipex Union (ANR-10-EQPX-52-01), the Labex NIE projects (ANR-11-LABX-0058 NIE) and CSC (ANR-10-LABX-0026 CSC) within the Investissement d’Avenir program ANR-10-IDEX-0002-02, RYSQ, as well as the NSF (PIF-1211914 and PFC-1125844), EOARD (FA8655-13-1-3032) and the Austrian Science Fund (FWF) via the project P24968-N27. Computations made use of the Janus supercomputer, supported by NSF (CNS-0821794), NCAR and CU Boulder/Denver.

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Contributions

T.W.E. conceived the idea and supervised the project. T.W.E. and E.O. designed the device experiments. J.G., J.A.H. and E.D. undertook the spectroscopic experiments. E.D., E.O., J.G., J.A.H. and J.F.D. fabricated and performed the device experiments. B.D., P.S., C. Genet and F.S. helped with the interpretation of the experimental data. G.P., C. Genes and J.S. developed the theoretical framework and performed the simulations. All authors contributed to the discussions and the preparation of the manuscript.

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Correspondence to T. W. Ebbesen.

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Orgiu, E., George, J., Hutchison, J. et al. Conductivity in organic semiconductors hybridized with the vacuum field. Nature Mater 14, 1123–1129 (2015). https://doi.org/10.1038/nmat4392

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