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Very large electro-optic responses in H-bonded heteroaromatic films grown by physical vapour deposition

Nature Materials volume 3, pages 910–917 (2004)Cite this article

Abstract

A crucial goal for modern telecommunications systems is development of very high-speed components for broadband (>100 GHz), all-optical signal/information processing. The core component of such technologies is the electro-optic modulator, which encodes electrical signals onto fibre-optic transmissions. A significant challenge therefore is obtaining materials that have large electro-optic responses and that can be readily fabricated into devices at low cost. We report here on the realization of high-response heteroaromatic organic chromophores that can be straightforwardly self-organized from the vapour phase into intrinsically acentric, high-quality, micrometre-scale films. These π-conjugated electro-optically active films (with second-order susceptibilities up to ∼100 pm V−1) are thermally stable and conveniently grown by a simple physical vapour deposition process in a few hours. Supramolecular acentricity is achieved without electric field poling, enforced by biomimetic heterocycle–hydroxycarbonyl head-to-tail hydrogen-bonding.

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Figure 1
Figure 2: Thermal analysis data for chromophores 1 (blue), 2 (red), and 3 (black).
Figure 3: Preparative pathways to films of type F1–F3.
Figure 4: Transmission optical absorption data for chromophores 1 (blue), 2 (red), and 3 (black).
Figure 5: Transmission polarized SHG spectroscopy.
Figure 6: Optical quality of H-bonded F2(1) films.
Figure 7: Chromophore polar orientation and microstructural stability.
Figure 8: Contact-mode AFM images of F2(1) films.

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Acknowledgements

We thank DARPA/ONR (SP01P7001R-A1/N00014-00-C), the NSF MRSEC program (DMR 0076077), and INSTM for financial support. E.A. thanks CNR for a postdoctoral fellowship. We also thank A. Abbotto and H. Kang for discussions, P. Dutta and G. Evmenenko for XRR data, and S.-T. Ho and Z. Liu for preliminary electro-optic coefficient measurements.

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Authors and Affiliations

  1. Department of Chemistry and the Materials Research Center, Northwestern University, Evanston, 60208-3113, Illinois, USA

    Antonio Facchetti, Elisabetta Annoni, Peiwang Zhu & Tobin J. Marks

  2. Department of Material Science, University of Milano-Bicocca, via Cozzi 53, Milano, 20125, Italy

    Luca Beverina, Marika Morone & Giorgio A. Pagani

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  1. Antonio Facchetti
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  2. Elisabetta Annoni
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Correspondence to Tobin J. Marks or Giorgio A. Pagani.

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Facchetti, A., Annoni, E., Beverina, L. et al. Very large electro-optic responses in H-bonded heteroaromatic films grown by physical vapour deposition. Nature Mater 3, 910–917 (2004). https://doi.org/10.1038/nmat1259

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