We investigated nonlinear absorption and photobleaching processes in a liquid-crystal elastomer doped with light-sensitive azobenzene moiety. A conventional one-dimensional holographic grating was recorded in the material with the use of two crossed UV laser beams and the angular dependence of the diffraction efficiency in the vicinity of the Bragg peak was analyzed. These measurements gave information on the depth to which trans to cis isomerization had progressed into the sample as a function of the UV irradiation time. Using a numerical model that takes into account the propagation of writing beams and rate equations for the local concentration of the absorbing trans conformer, we computed the expected spatial distribution of the trans and cis conformers and the shape of the corresponding Bragg diffraction peak for different irradiation doses. Due to residual absorption of the cis conformers the depth of the recording progresses logarithmically with time and is limited by the thermal relaxation from the cis to trans conformation.
The optical mechanism for imprinting one-dimensional grating structures into thin films of a light-sensitive monodomain liquid crystal elastomer is investigated by analyzing the time dependence of optical diffraction properties. The recording kinetics shows an irregular oscillatory behavior, which is most expressed at small grating spacings and at temperatures close to the nematic-isotropic phase transition. The oscillations are attributed to the opto-mechanical response of the film, i.e., to contraction of the film during the recording process. At temperatures far below the nematic-isotropic phase transition, the spontaneous erasure kinetics exhibits exponential relaxation with relaxation time following the Arrhenius activation law. However, at temperatures close to the nematic-isotropic phase transition, the erasure process shows an interesting nonmonotonic behavior that we attribute to the non-linear relation between the concentration of the photo-transformed chemical groups and the nematic order parameter.
We investigate light-induced patterning of a monodomain side-chain liquid crystal elastomer (SC-LCE) doped with light-sensitive azobenzene moiety in the temperature region close to the nematic-paranematic phase transition. We show that a strongly nonlinear relationship between the concentration of the cis isomers of the azomesogens and the refractive index modification of the material, which is characteristic for the phase transition region, results in nonmonotonous time dependence of the diffraction efficiency of a probe beam. From this effect we determine the sensitivity of the nematic transition temperature on the molar fraction of the cis isomers. The relation between the cis isomer molar fraction and nematic order also provides a possibility for recording hidden holograms, which can be made visible by cooling the sample from the paranematic to the nematic phase.
An appealing property of optical diffractive structures from elastomeric materials is a possibility to regulate their optical patterns and consequently also their diffractive features with mechanical straining. We investigated the effect of strain on diffraction characteristics of holographic gratings recorded in a monodomain side-chain liquid crystalline elastomer. The strain was imposed either parallel or perpendicular to the initial alignment direction of the material. At temperatures far below the nematic-paranematic phase transition, straining along the initial alignment affects mainly the diffraction pattern, while the diffraction efficiency remains almost constant. In contrast, at temperatures close to the nematic-paranematic phase transition, the diffraction efficiency is also significantly affected. Straining in the direction perpendicular to the initial alignment strongly and diversely influences both the diffraction pattern and the diffraction efficiency. The difference between the two cases is attributed to shear-stripe domains, which form only during straining perpendicular to the initial alignment and cause optical diffraction that competes with the diffraction from the holographic grating structure.
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