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. |
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Current activities
Towards unusual Bragg reflection properties:
How to broaden the light reflection band of cholesteric
lcs ?
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What is well known by the Liquid Crystal Physicist:
the selective light reflection in cholesteric liquid crystals
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| 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).
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| 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:
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:
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.
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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).
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| I.
Why and how to broaden the wavelength bandwidth in clcs ? |
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| 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
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| II.
How to go beyond the 50% limit of reflectance of cholesteric lcs
? |
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| 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.
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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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