We report the first observation of the photorefractive effect in a polymeric material, the electro-optic polymer bisphenol-A-diglycidylether 4-nitro-1,2-phenylenediamine made photoconductive by doping with the hole-transport agent diethylamino-benzaldehyde diphenylhydrazone. The gratings formed exhibit dynamic writing and erasure, strong electric-field dependence, polarization anisotropy, and estimated space-charge fields up to 26 kV/cm at an applied field of 126 kV/cm. Application of similar concepts should provide a broad new class of easily fabricated photorefractive materials.

/pdf/observation-of-the-photorefractive-effect-in-a-polymer-2bn27m3my1.pdf

Observation of the photorefractive effect in a polymer.

Stable polymeric materials for nonlinear optics: a review based on azobenzene systems

Piezoelectric properties of polymeric substances arise from either the poling-induced orientation of molecular dipoles (class 1) or the uniaxial orientation of chiral chain molecules (class 2). The class 1 polymers include ferroelectric polymers, polar polymers with frozen-in dipole orientation, and the composites of polymers with ferroelectric ceramics. Details of the poling procedure in representative materials are described, and optimum poling conditions are suggested. Resulting piezoelectric and pyroelectric activities are specified as a function of remnant polarization, and underlying basic mechanisms are summarized. The class 2 polymers consist of drawn optically active polymers and exhibit face-shear piezoelectricity appearing in proportion to the orientation coefficient of chain axes. The spontaneous polarization of ferroelectric liquid-crystalline polymers is attributable to this type of piezoelectricity coupled with the spontaneous strain. >

Piezoelectricity and pyroelectricity in polymers

Polar orientation of molecules in solids leads to materials with potentially useful properties such as nonlinear optical and electrooptical activity, electrochromism, and pyroelectricity. A simple self-assembly procedure for preparing such materials is introduced that yields multiple polar dye monolayers on solid surfaces joined by zirconium phosphate-phosphonate interlayers. Second harmonic generation (SHG) shows that the multilayers have polar order that does not decrease with increasing numbers (up to a large number) of monolayers in the film. The inorganic interlayers, as determined by SHG, impart excellent orientational stability to the dye molecules, with the onset of orientational randomization above 150°C.

https://science.sciencemag.org/content/sci/254/5037/1485.full.pdf

Polar orientation of dyes in robust multilayers by zirconium phosphate-phosphonate interlayers.

A new class of electro-optic chromophores, of which 2-dicyanomethylen-3-cyano-4-{2-[ E -(4- N , N -di(2-acetoxyethyl)-amino)-phenylene-(3,4-dibutyl)thien-5]- E -vinyl}-5,5-dimethyl-2,5-dihydrofuran (denoted FTC) is the prototype, has been prepared, characterized, and used to fabricate electro-optic devices. The molecular hyperpolarizability and thermal stability of these chromophore molecules are exceptional. Strong intermolecular electrostatic interactions inhibit the efficient poling of these molecules. A statistical mechanical theoretical treatment is used to quantitatively predict the competition of poling, intermolecular electrostatic interactions, and thermal effects in defining achievable acentric order and hence macroscopic optical nonlinearity. Theory is used to predict the optimum chromophore structure and material composition (chromophore loading in a polymer matrix) for maximum electro-optic activity and minimum optical loss. Problems associated with lattice hardening to lock-in poling-induced order are discussed briefly.

The molecular and supramolecular engineering of polymeric electro-optic materials

Extending the novel method of Eich et al. [J. Appl. Phys. 66, 3241 (1989)] to prepare highly stable second‐order nonlinear optical (NLO) polymers via chemical cross‐linking under electric field, we have obtained a new polymer exhibiting large and stable second‐order optical nonlinearities after relaxation at 80 °C. This was achieved by forming a network polymer from two NLO‐active monomers, bifunctional N,N‐(diglycidyl)‐4‐nitroaniline and trifunctional N‐(2‐aminophenyl)‐4‐nitroaniline. Here, every NLO moiety is connected to the network by a single covalent bond. After full cure under corona poling at 120 °C, the sample exhibited at ambient conditions d33≂50 pm/V and d31≂16 pm/V at 1064 nm fundamental wavelength, as estimated from the Maker fringe data. Upon heating to 80 °C, the nonlinearities decreased somewhat initially, but leveled off and remained stable at 80 °C. This stable sample gave d33≂42 pm/V and d31≂14 pm/V at ambient conditions. Furthermore, the linear electro‐optical coefficient of this samp...

Highly efficient and stable nonlinear optical polymers via chemical cross‐linking under electric field

Liquid-crystalline polyesters with cholesteric and probably chiral smectic C∗ phases were prepared using combined liquid-crystalline polymers (that is polymers with the mesogenic groups in the main chain as well as in the side groups). Copolyesters of these polymers and polymers with olefinic double bonds could be cross-linked retaining the liquid-crystalline phases. This resulted in cross-linked polymers with elastic properties.

New liquid-crystalline polymers with chiral phases

Relation pour des polymeres a groupe lateral cristal liquide. Synthese de cristaux liquides elastomeres a partir de cristaux liquides polymeres

Structure‐property relations in linear and crosslinked liquid crystalline polymers

New polymeric thin films containing nonlinear optical chromophores aligned by corona poling for χ (2) experiments have been monitored by spectroscopic and optical waveguiding techniques, as well as by second harmonic generation and electrooptic measurements. Stability has been improved considerably in various crosslinked epoxy polymers by attaching the chromophores at several molecular positions to inhibit relaxation. With increased chromophore concentration and improved alignment, films exhibiting nonlinearities exceeding lithium niobate have now been demonstrated. Several electrooptic phase modulators have been constructed with these new materials and some preliminary results are presented.

Poled Epoxy Polymers for Optoelectronics

A variety of optically nonlinear tolan chromophores and epoxy based polymers containing them have been prepared and studied. The molecular hyperpolarizabilities of the dye chromophores have been me...

Nonlinear Optical Epoxy Polymers with Polar Tolan Chromophores

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