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We compare the photochemical stability of the nonlinear optical chromophore configurationally locked polyene 2-{3-[2-(4-dimethylaminophenyl)vinyl]-5,5-dimethylcyclohex-2-enylidene} malononitrile (DAT2) embedded in a polymeric matrix and in a single-crystalline configuration. The results show that, under resonant light excitations, the polymeric compound degrades through an indirect process, while the DAT2 crystal follows a slow direct process. We show that chromophores in a crystalline environment exhibit three orders of magnitude better photostability as compared to guest-host polymer composites.

Organic nonlinear optical materials have proven to possess high and extremely fast nonlinearities compared to conventional inorganic crystals, allowing for sub-1-V driving voltages and modulation bandwidths of over 100 GHz. Compared to more widely studied poled electro-optic polymers, organic electro-optic crystals exhibit orders of magnitude better thermal and photochemical stability. The lack of available structuring techniques for organic crystals has been the major drawback for exploring their potential for photonic structures. Here we present a new approach to fabricate high-quality electro-optic single crystal waveguides and nanowires of configurationally locked polyene DAT2 (2-(3-(2-(4-dimethylaminophenyl)vinyl)-5,5-dimethylcyclohex-2-enylidene)malononitrile). The high-index-contrast waveguides (delta(n) = 0.54 +/- 0.04) are grown from the melt between two anodically bonded borosilicate glass wafers, which are structured and equipped with electrodes prior to bonding. Electro-optic phase modulation is demonstrated for the first time in the non-centrosymmetric DAT2 single crystalline channel waveguides at a wavelength of 1.55 microm. We also show that this technique in combination with DAT2 material allows for the fabrication of single-crystalline nanostructures inside large-area devices with crystal thicknesses below 30 nm and lengths of above 7 mm.

High quality organic electro‐optic single crystalline thin films are produced on amorphous C≡N‐modified glass substrates (see figure), which is a mimic surface of a crystal, by slow evaporation and capillary methods. The films have a suitable size (shaped as rectangular plates with side lengths in the range of 5–10 mm and regular thicknesses in the range of 1–40 μm) for the fabrication of photonic devices.