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PHOTONIC BAND STRUCTURES
Broadband cholesteric reflectors

Research area

Our current research activities deal with cholesteric and chiral nematic liquid crystals (lcs): low molar mass lcs, glassy mesomorphic oligomers, crosslinked mesomorphic polymers with a peculiar attention devoted to Polymer-Stabilized LCs – also called anisotropic gels, for which a polymer network is created in the lc volume by UV light induced polymerization. In relation with the experimental conditions, the relevant scale of the structure and properties of the final material is the nanometer or micrometer scale. Polymer-Stabilized LCs are also called LC nanocomposites or microcomposites.

We study the relation between the conditions of the material design – formulation of mixtures, UV light curing, thermal history, etc. –, the optical and electro-optical properties – Bragg light reflections – and the structure as investigated by transmission electron microscopy, scanning electron microscopy or near-field microscopies.

 


Current activities


Towards unusual Bragg reflection properties:
How to broaden the light reflection band of cholesteric lcs ?

What is well known by the Liquid Crystal Physicist:
the selective light reflection in cholesteric liquid crystals

The cholesteric lc structure. Cholesteric liquid-crystalline states of matter are widely present in nature: atherosclerosis, arthropods cuticles, condensed phases of DNA, plant cell walls, human compact bone osteon, chiral biopolymers, etc. The self organized helical structure produces unique optical properties. The elongated chiral molecules of a cholesteric lc exhibit a long-range orientational order which presents a twisted arrangement in a direction perpendicular to their long axis; in a parallel direction, the structure is similar to the nematic lc one, i.e.: the molecules are on average parallel together without any positional order. Therefore the director of the molecules rotates around a helical axis and the distance over which it rotates 360° is called the pitch.


Light reflection from the cholesteric helical structure
(by permission from Nature 391, 745-746, copyright 1998 Macmillan Publishers Ltd).

Property of selective light reflection by a cholesteric lc. Cholesteric lcs exhibit many remarkable properties due to the existence of the macroscopic helical structure. The most striking features are the exceptionnally large optical rotatory power and the iridescent colours due to the selective reflection displayed by a uniformly oriented Grandjean planar texture, when the helix axis is perpendicular to the observation plane. At normal incidence, the mean reflection wavelength λ0 is related to the pitch p and the mean refraction index n by:

λ0 = np

n is the average of the ordinary (n0) and the extraordinary of (ne) refractive indices of the locally uniaxial structure : n = (n0 + ne)/2. The spectral width of the reflection band Δλ is defined as:

Δλ = pΔn

where Δn = ne - n0 is the birefringence. Within Δλ, an incident unpolarized or linearly polarized light beam parallel to the helix axis is split into two opposite circularly polarized components, one of which is transmitted whereas the other is reflected. The sense of rotation of the latter one agrees with the helix screw sense. A wavelength out of Δλ is simply transmitted.

Compared to conventional pigmented color filters, a clc slab has the special feature to combine several optical properties in one layer: it is not only a filter but also a reflector and a polarizer. Since Δn is limited to 0.3 – 0.4 for colourless organic compounds: the bandwidth Δλ is limited to a few tens of nm in the visible spectrum (see below the related contribution n°I from CEMES on this matter).

Therefore the reflected light is circularly polarized with the same handedness as the

incident light, which is the exact opposite of a normal dielectric mirror that changes the handedness.For example, right-handed circularly polarized incident light is reflected by a right-handed helix and, in contrast, if left-handed circularly polarized, the incident light is transmitted without significant loss through the medium. Consequently, as only circularly polarized light with one handedness is reflected, the reflected intensity of ambient unpolarized light from a CLC is never greater than 50% (see below the related contribution n°II from CEMES on this matter).



I. Why and how to broaden the wavelength bandwidth in clcs ?
 

However huge the choice is for pitch values, Δn is typically limited to 0.3-0.4 for colourless organic materials. As a consequence, Δλ is commonly less than 100 nm in the visible spectrum and more often around 50 nm.

Whereas the selectivity is desirable for several families of applications (narrow-band optical filters, thermal imaging, laser or paint technologies), a drawback lies in the fact that known cholesteric filters have a too limited reflection bandwidth for specific purposes like full-colour or white-or-black polariser-free reflective displays, broadband circular polarisers or smart windows in buildings for which the solar control would be required over a broad wavelength band. From fundamental considerations, it is thus challenging to increase the reflection bandwidth by finding novel helical structures, with a non-monotonous spatial distribution of the periodicity, and to investigate how the optical response of the material has to be revised.

Below is a selected number of results from CEMES on the subject of broadband reflective cholesteric structures:

  • Polymer-Stabilized Cholesteric LCs elaborated out of thermodynamical equilibrium conditions. By combining the UV light curing with a thermally-induced pitch variation, memory effects are introduced into the characteristics of the reflection band of the material at room temperature. In the visible spectrum, the reflection bandwidth can be tuned in agreement with the thermal ramp and broadened.
  • In addition, the bandgap filters can be switched between broadband reflective, scattering and transparent states by subjecting them to an electric field.
    Related papers: [5] and [6] in Selected publications

  • Polymer-Stabilized Cholesteric LCs for which the UV light is screened during the elaboration. The UV light absorbing properties of the LC constituent may induce the broadening of the reflection bandwidth of the gel, which situation is promoted by asymmetrical irradiation conditions (only one side of the cell is irradiated). The in situ structure of the polymer network, included in the LC, is investigated by transmission electron microscopy and the temperature-dependence of the reflection properties is examined. This result is discussed in relation with the variation of the reflection band characteristics with the polymer concentration, which offers the opportunity to have an indirect access to the volume distribution of the cholesteric periodicities.

    Related paper: [10] in Selected publications

  • Glassy cholesteric LCs from an anisotropic thermal diffusion in a bilayer film

    Related papers: [8] and [9] in Selected publications


  •  
    II. How to go beyond the 50% limit of reflectance of cholesteric lcs ?
     

    At CEMES, we found the elaboration procedure of a cholesteric gel whose the optical characteristics go beyond the 50% reflectance limit. Photopolymerizable monomers are introduced in the volume of a clc exhibiting a thermally induced helicity inversion and the blend is then cured with UV light when the helix is right-handed. The reflectance exceeds 50% when measured at the temperature assigned at a cholesteric helix with the same pitch but a left-handed sense before reaction. The reflection properties are investigated in the infrared region. From scanning electron microscopy investigations, we have shown that the organization of the mesophase is transferred onto the structure of the network. The gel structure was discussed as consisting of a polymer network with a helical structure containing two populations of low molar mass LC molecules. Each of them was characterized by a band of circularly polarized light which is selectively reflected. The monitoring of the optical response with the temperature offers the opportunity to discriminate the respective contributions of bound and free fraction of lc molecules to the reflectance and to give evidence of the progressive increase of the reflected flux when the temperature decreases from the curing temperature. Novel opportunities to modulate the reflection over the whole range are offered. Potential applications are related to the light management for smart windows or reflective polarizer-free displays with a larger scale of reflectivity levels.


    Scanning electron microscopy image of the polymer network formed in the cholesteric phase. The helical structure has been transferred onto the polymer morphology. The polymer fibrils draw stacked rows of parallel arcs which appear when the cut direction is oblique to the helical axis; these arcs are enhanced in white on the left part of the picture. Such arced patterns are also visible in thin sections of biological materials: crustacean integuments, dermal plates of fishes, insect cuticles, collageneous matrices of bone tissue, plant cell walls and chromatin organizations for DNA.

    The case of Plusiotis Resplendens
    Click above to know more about this charming beetle for which the reflectance limit is no more valid.

    Related papers: [11] and [12] in Selected publications

     

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