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Organic Phenolic Configurationally Locked Polyene Single Crystals for Electro-optic and Terahertz Wave Applications†

  1. O-Pil Kwon1,2,*,
  2. Seong-Ji Kwon1,
  3. Mojca Jazbinsek1,
  4. Fabian D. J. Brunner1,
  5. Jung-In Seo3,
  6. Christoph Hunziker1,
  7. Arno Schneider1,
  8. Hoseop Yun4,
  9. Yoon-Sup Lee3,
  10. Peter Günter1

Article first published online: 29 SEP 2008

DOI: 10.1002/adfm.200800633

Issue

Advanced Functional Materials

Advanced Functional Materials

Volume 18, Issue 20, pages 3242–3250, October 23, 2008

Additional Information

How to Cite

Kwon, O.-P., Kwon, S.-J., Jazbinsek, M., Brunner, F. D. J., Seo, J.-I., Hunziker, C., Schneider, A., Yun, H., Lee, Y.-S. and Günter, P. (2008), Organic Phenolic Configurationally Locked Polyene Single Crystals for Electro-optic and Terahertz Wave Applications. Advanced Functional Materials, 18: 3242–3250. doi: 10.1002/adfm.200800633

Author Information

  1. 1

    Nonlinear Optics Laboratory, ETH Zurich 8093 Zurich (Switzerland)

  2. 2

    Department of Molecular Science and Technology, Ajou University Suwon 443-749 (Korea)

  3. 3

    Department of Chemistry and School of Molecular Science (BK 21) Korea Advanced Institute of Science and Technology (KAIST) Daejeon 305-701 (Korea)

  4. 4

    Division of Energy Systems Research and Department of Chemistry, Ajou University Suwon 443-749 (Korea)

*Nonlinear Optics Laboratory, ETH Zurich 8093 Zurich (Switzerland).

  1. †

    We thank J. Hajfler for the polishing of OH1 samples. This work has been supported by the Swiss National Science Foundation and the Korea Foundation for International Cooperation of Science & Technology (KICOS) through a grant provided by the Korean Ministry of Science & Technology(MOST) (No. 2007-00440).

Publication History

  1. Issue published online: 21 OCT 2008
  2. Article first published online: 29 SEP 2008
  3. Manuscript Received: 7 MAY 2008

Funded by

  • Swiss National Science Foundation
  • Korean Ministry of Science & Technology(MOST). Grant Number: 2007-00440

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Keywords:

  • crystal growth;
  • electron transport;
  • electro-optical materials;
  • nonlinear optical materials

Graphical Abstract

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Configurationally locked polyene OH1 crystals containing a phenolic electron donor exhibit large second-order nonlinear optical figures of merit, high thermal stability, and very favorable crystal-growth characteristics. A very high potential of OH1 crystals for broadband THz wave emitters in the full frequency range of 0.1–3 THz by optical rectification of 160 fs pulses has been demonstrated.

Abstract

We investigate a configurationally locked polyene (CLP) crystal 2-(3-(4-hydroxystyryl)-5,5-dimethylcyclohex-2-enylidene)malononitrile (OH1) containing a phenolic electron donor, which also acts as a hydrogen bond donor. The OH1 crystals with orthorhombic space group Pna21 (point group mm2) exhibit large second-order nonlinear optical figures of merit, high thermal stability and very favorable crystal growth characteristics. Higher solubility in methanol and a larger temperature difference between the melting temperature and the decomposition temperature of OH1 compared to analogous CLP crystals, are of advantage for solution and melt crystal growth, respectively. Acentric bulk OH1 crystals of large sizes with side lengths of up to 1 cm with excellent optical quality have been successfully grown from methanol solution. The microscopic and macroscopic nonlinearities of the OH1 crystals are investigated theoretically and experimentally. The OH1 crystals exhibit a large macroscopic nonlinearity with four times larger powder second harmonic generation efficiency than that of analogous CLP crystals containing dimethylamino electron donor. A very high potential of OH1 crystals for broadband THz wave emitters in the full frequency range of 0.1–3 THz by optical rectification of 160 fs pulses has been demonstrated.

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