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Organic Phenolic Configurationally Locked Polyene Single Crystals for Electro‐optic and Terahertz Wave Applications
Authors:O‐Pil Kwon  Seong‐Ji Kwon  Mojca Jazbinsek  Fabian D. J. Brunner  Jung‐In Seo  Christoph Hunziker  Arno Schneider  Hoseop Yun  Yoon‐Sup Lee  Peter Günter
Affiliation:1. Nonlinear Optics Laboratory, ETH Zurich 8093 Zurich (Switzerland);2. Department of Molecular Science and Technology, Ajou University Suwon 443‐749 (Korea);3. Department of Chemistry and School of Molecular Science (BK 21) Korea Advanced Institute of Science and Technology (KAIST) Daejeon 305‐701 (Korea);4. Division of Energy Systems Research and Department of Chemistry, Ajou University Suwon 443‐749 (Korea)
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.
Keywords:crystal growth  electron transport  electro‐optical materials  nonlinear optical materials
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