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Passive and active polarization elements were created by surface and bulk photo-alignment of LCs, reactive LCs, photo-sensitive LCP and photo-curable monomer/LC composites. The use of different photo-sensitive liquid crystalline materials for the development of highly anisotropic elements with high spatial resolution and stability or, alternatively, fast switch ability will be discussed. Photo-active and voltage tunable polarization and diffraction elements are presented. For active micro-optic application a photo-addressed patterned retarder was created. Electrically switchable diffraction gratings were generated by interference exposure of photo-curable LC composites at room temperature characterized by droplet free morphology. These polarization sensitive diffraction elements are characterized be excellent optical properties and low switching times.
The past two decades witnessed tremendous progress in the field of creation of different types of responsive materials. Cholesteric polymer networks present a very promising class of smart materials due to the combination of the unique optical properties of cholesteric mesophase and high mechanical properties of polymer networks. In the present work we demonstrate the possibility of fast and reversible photocontrol of the optical properties of cholesteric polymer networks. Several cholesteric photopolymerizable mixtures are prepared, and porous cholesteric network films with different helix pitches are produced by polymerization of these mixtures. An effective and simple method of the introduction of photochromic azobenzene-containing nematic mixture capable of isothermal photoinducing the nematic isotropic phase transition into the porous polymer matrix is developed, It is found that cross-linking density and degree of polymer network filling with a photochromic nematic mixture strongly influence the photo-optical behavior of the obtained composite films. In particular, the densely cross-linked films are characterized by a decrease in selective light reflection bandwidth, whereas weakly cross-linked systems display two processes: the shift of selective light reflection peak and decrease of its width. It is noteworthy that the obtained cholesteric materials are shown to be very promising for the variety applications in optoelectronics and photonics.
Effective volume holographic structures based on organic-inorganic photopolymer nanocomposites
(2009)
We demonstrate a practical approach for the development of a broad range of nanocomposites based on acrylate polymers and organically capped inorganic nanoparticles (NPs). The submicrometer scale volume patterning of the nanocomposites using holographic photopolymerization was investigated. The specific adjustment of both the material parameters (core-shell of the NP, monomer mixture, concentrations) and the patterning conditions led to materials that were suitable for the fabrication of effective optical diffractive elements and specific functional microdevices with light-emissive and nonlinear optical (NLO) properties. The nanocomposite preparation and properties, their holographic performance and some examples of functional polymer-NP structures are reported.
For the first time the cholesteric mixture containing nematic polymer with small amount of chiral-photochromic dopant is used for electroinduced diffraction gratings production. The gratings are obtained by applying electric field to the planar-aligned cholesteric polymer layer causing its periodical distortion. Material developed permits manipulating supramolecular helical structure by means of UV exposure resulting in helix untwisting. Photo-controlling of helix pitch brings to change parameters of the electroinduced gratings. Due to macromolecular "nature" of the material one can easily stabilize electroinduced gratings by fast sample cooling. All-known cholesteric grating types are realized in the studied polymer material. It is observed that the grating vector can be oriented along or perpendicular to the rubbing direction of the cell. It is shown that the diffraction efficiency is dictated by grating type and the amplitude of the applied electric field and can achieve about 80%. Moreover, the period of gratings can be tuned upon UV light illumination. The possibility of 2D gratings creation is also demonstrated. The described material and approach gives an opportunity to easily fabricate a variety of diffraction gratings with flexibly controllable parameters. Such gratings can be potentially applied in optics, optoelectronics, and photonics as intelligent diffraction elements.
We studied peculiarities of the structural reconstruction within holographically recorded gratings on the surface of several different amorphous azobenzene-containing polymers. Under illumination with a light interference pattern, two processes take place in this type of polymer. The first process is the light-induced orientation of azobenzene units perpendicular to the polarization plane of the incident light. The second one is a transfer of macromolecules along the grating vector (i.e. perpendicular to the grating lines). These two processes result in the creation of a volume orientation grating (alternating regions of different direction or degree of molecular orientation) and a surface relief grating (SRG)-i.e. modulation of film thickness. One can assume that both orientation of molecules and their movement might change the local mechanical properties of the material. Therefore, formation of the SRG is expected to result also in modulation of the local stiffness of the polymer film. To reveal and investigate these stiffness changes within the grating, spin-coated polymer films were prepared and the gratings were recorded on them in two different ways: with an orthogonal circular or orthogonal linear polarization of two recording light beams. A combination of atomic force microscopy (AFM) and ultrasonic force microscopy (UFM) techniques was applied for SRG development monitoring. We demonstrate that formation of the phase gratings depends on the chemical structure of polymers being used, polymer film thickness, and recording parameters, with the height of grating structures (depth of modulation) increasing with both the exposure time and the film thickness. UFM images suggest that the slopes of the topographic peaks in the phase gratings exhibit an increased stiffness with respect to the grating depressions.
A new type of self-organized materials based on cholesteric networks filled with photoactive side-chain copolymer is being developed. Supramolecular helical structure of cholesteric polymer network resulting in the selective reflection is used as a photonic scaffold. Photochromic azobenzene-containing nematic copolymer is embedded in cholesteric scaffold and utilized as a photoactive media for optical pattering. 1D and 2D transmission diffraction gratings are successfully recorded in composite films by holographic technique. For the first time the possibility to create selective reflection gratings in cholesteric material mimicking the natural optical properties of cholesteric mesophase is demonstrated. That enables the coexistence of two selective gratings, where one has an intrinsic cholesteric periodic helical structure and the other is a holographic grating generated in photochromic polymer. The full-polymer composites provide high light-induced optical anisotropy due to effective photo-orientation of side-chain fragments of the azobenzene-containing liquid crystalline polymer, and prevent the degradation of the helical superstructure maintaining all optical properties of cholesteric mesophase. The proposed class of optical materials could be easily applied to a broad range of polymeric materials with specific functionality. The versatility of the adjustment and material preprogramming combined with high optical performance makes these materials a highly promising candidate for modern optical and photonic applications.
Synthesis, self-organization, and optical properties of supermolecular tripedal liquid crystals incorporating various prototypical mesogenic units such as alkoxy-azobenzene (AZB), alkoxy-biphenylene (BPH) or alkoxy-cyanobiphenyl (OCB) derivatives are reported. Different molecular systems were designed in order to sequentially incorporate the smectogenic-like alkoxy-azobenzene-based chromophore within the molecular structure, whose relative proportion is selectively varied by exchanging with the other mesogens. A divergent synthetic mode was elaborated for their synthesis, starting from the regioselective functionalization of the phloroglucinol-based (PG) inner core. This methodology allowed the preparation of several sets of unconventional tripedal oligomers with conjugated heterolithic structures (made of different blocks, e.g. PG(6)AZB(x)BPH(3-x) and PG(6)AZB(x)OCB(3-x), x = 1 or 2) along the homolithic parents (all identical blocks, e.g. PG(z)AZB(3), z = 6 or 11, z is the number of methylene in the spacer between PG and the protomesogen, PG(6)BPH(3), and PG(6)OCB(3)), respectively. Essentially all the synthesized systems behave as thermotropic liquid crystals and show various types of highly segregated multilayered smectic phases, or, in one case, a nematic phase, depending on the nature of the constitutive anisotropic blocks and on the molecular topology (homolithic versus heterolithic, mesogenic ratio x : 3 - x). The effects of these structural modifications on the mesomorphism (mesophase structures, temperature ranges, and thermodynamic stability) have been investigated by differential scanning calorimetry and small-angle X-ray diffraction experiments combined with dilatometric measurements. Models describing the various supramolecular organizations of these tripedes into such multilayered structures are proposed and discussed. Preliminary results of the investigations of their optical properties will also be presented.
The structure and morphology on different length scales dictate both the electrical and optical properties of organic semiconductor thin films. Using a combination of spectroscopic methods, including scanning near-field optical microscopy, we study the domain structure and packing quality of highly crystalline thin films of oligomeric PQT-12 with 100 nanometer spatial resolution. The pronounced optical anisotropy of these layers measured by polarized light microscopy facilitates the identification of regions with uniform molecular orientation. We find that a hierarchical order on three different length scales exists in these layers, made up of distinct well-ordered dichroic areas at the ten-micrometer-scale, which are sub-divided into domains with different molecular in-plane orientation. These serve as a template for the formation of smaller needle-like crystallites at the layer surface. A high degree of crystalline order is believed to be the cause of the rather high field-effect mobility of these layers of 10(-3) cm 2 V(-1) s(-1), whereas it is limited by the presence of domain boundaries at macroscopic distances.
Threshold reduction and emission enhancement are reported for a gold nanoparticle-based waveguided random laser, exploiting the localized surface plasmon resonance excitation. It was experimentally found that a proper thickness of the spacer layer between the gold nanoparticles and the gain layer enhances the random laser performance. It tunes the coupling between the gain polymer and the gold nanoparticles and avoids the quenching of emission in close contact to the gold nanoparticles which is considered as one of the main sources of loss in the current laser system. (C) 2013 American Institute of Physics. [http://dx.doi.org/10.1063/1.4800776]
Metal ion mediated mesomorphism and thin film behaviour of amphitropic tetraazaporphyrin complexes
(2001)
We report on the influence of localized surface plasmon resonance excitation of Au@SiO2 core-shell nanoparticles on the amplified spontaneous emission of a semiconductor polymer composite (F8BT/MEH-PPV). Au@SiO2 nanoparticles are compatible with the donor-acceptor polymer matrix and get uniformly distributed within the whole polymer film. The plasmon resonance band of the nanoparticles correlates with both the emission and excitation spectra of the polymer composite, as well as with the donor emission and acceptor excitation spectra. We demonstrate that resonantly excited Au@SiO2 nanoparticles enhance the amplified spontaneous emission and the modal gain of the polymer films. The measurement of influential factors reveals that the emission is enhanced predominantly by the increase of acceptor excitation rate, which is accompanied by depletion of the FRET efficiency and increase of quantum yield. The enhancement factor is increased by both introducing a higher loading of plasmonic nanoparticles in the polymer film and increasing the excitation energy. This work shows that these plasmonic nanoantennas are able to enhance the stimulated emission of semiconductor polymers by improving the size mismatch between the excitation light and the emitting polymer.