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Dielectric relaxation study of a H
shaped liquid crystal dimer
Abhishek Kumar Misra
a
, Satya Prakash Yadav
a
, Pankaj Kumar
Tripathi
a
, Rajiv Manohar
a
, Ashish K. Prajapati
b
& Mahesh C.
Varia
b
a
Liquid Crystal Research Lab, Physics Department, University of
Lucknow, Lucknow 226007, India
b
Applied Chemistry Department, Faculty of Technology and
Engineering, The M.S. University of Baroda, Vadodara 390 001,
India
Version of record first published: 13 Jul 2012.
To cite this article: Abhishek Kumar Misra, Satya Prakash Yadav, Pankaj Kumar Tripathi, Rajiv
Manohar, Ashish K. Prajapati & Mahesh C. Varia (2012): Dielectric relaxation study of a H shaped
liquid crystal dimer, Physics and Chemistry of Liquids: An International Journal, 50:5, 605-616
To link to this article: http://dx.doi.org/10.1080/00319104.2011.651210
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Physics and Chemistry of Liquids
Vol. 50, No. 5, SeptemberOctober 2012, 605616
Dielectric relaxation study of a H shaped liquid crystal dimer
Abhishek Kumar Misra
a
, Satya Prakash Yadav
a
, Pankaj Kumar Tripathi
a
,
Rajiv Manohar
a
*
, Ashish K. Prajapati
b
and Mahesh C. Varia
b
a
Liquid Crystal Research Lab, Physics Department, University of Lucknow, Lucknow
226007, India;
b
Applied Chemistry Department, Faculty of Technology and
Engineering, The M.S. University of Baroda, Vadodara 390 001, India
(Received 5 August 2011; final version received 12 November 2011)
The present article reports dielectric relaxation study of an unusual shaped
liquid crystal dimer (H shape) in the temperature range 4085

C. The study
of this liquid crystal dimer is important due to the presence of azo central
linkage, which is photosensitive. The dielectric relaxation study indicates
coupling between the electric field and the liquid crystal molecule of H
shaped dimer. Various dielectric properties for this liquid crystal dimer are
quite different from the conventional liquid crystals. The dielectric
relaxation observed in the smectic phase is due to the reorientation of
molecule along the director in the presence of an applied electric field. The
temperature dependence of the dielectric parameters, such as relaxation
frequency, relaxation strength and distribution parameter have been
evaluated for this liquid crystal dimer for both planar as well as
homeotropically aligned cell and then compared. The ColeCole equation
has been used to evaluate the aforementioned parameters.
Keywords: relaxation frequency; dielectric parameters; liquid crystal dimer
1. Introduction
The molecular shape of liquid crystalline materials has been restricted to rod-like or
disk-like units for several decades. These basic shapes are rather easy for designing
nematic, smectic or columnar arrangements [13]. The inventive action of chemists
led to the synthesis of new shaped liquid crystalline materials with more anisotropic
properties and as a result of which, the new mesomorphic arrangements were
invented. The constituent molecules of the compounds that generate the liquid
crystalline phases are usually rod-like in nature [4]. However, these phases can also
be exhibited by materials that consist of bent-core molecules, provided that this bend
is not too acute and the molecular length is sufficient to overcome the destructive
nature of the bent-shape [46]. The conventional structure of liquid crystal is a rigid
core attached with flexible alkyl chains. The core provides the source of anisotropy
for the formation of liquid crystalline phases. However, disorder associated with the
terminal chains reduces the stability of solid crystal phases and allows the
appearance of liquid crystal phases. Some of the liquid crystal phases exhibited by
materials with molecules of unusual shapes, such as lambda shape, X shape, S shape,
*Corresponding author. Email: rajiv.manohar@gmail.com
ISSN 00319104 print/ISSN 10290451 online
2012 Taylor & Francis
http://dx.doi.org/10.1080/00319104.2011.651210
http://www.tandfonline.com
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are reported in the literature [3,4,7,8]. One of the interesting sub-fields of the liquid
crystals designing are liquid crystal dimer [9] with unusual shape [47]. The liquid
crystal dimers [9] have attracted much interest in recent years for both theoretical
and experimental research due to their unusual properties as compared to the
conventional liquid crystals. The liquid crystal dimers serve as a model compound
for semiflexible main chain liquid crystal polymers. Due to the increasing importance
of the liquid crystal dimers, studies have been carried out on these samples by
using various experimental techniques. Recently, Prajapati et al. [10] and Kumar
et al. [11,12] have reported synthesis and some properties of H-shaped liquid crystal
dimer.
The most important property that can vary due to the unusual shape of the liquid
crystal molecule is its dielectric anisotropy. It arises mainly due to their long-range
molecular ordering and affects the switching behaviour of the liquid crystals, which
in turn is strongly related to the applications of liquid crystals in the device
applications. The study of dielectric anisotropy of H shaped liquid crystal dimer is
the basis for the use in different devices, because it provides significant information
about the arrangement of the molecules within the system.
The present investigation is important because of the presence of a photosensitive
azo central linkage in the liquid crystal dimer [10]. The presence of azo central
linkage in the liquid crystal dimer makes it a promising material for the
photomechanical devices and image storing due to its high resolution and sensitivity.
The aim of this work is to study dielectric relaxation phenomena of H shaped liquid
crystal dimer. In addition to this relaxation time, relaxation strength, relative
permittivity, dielectric anisotropy have also been determined for this H shaped liquid
crystal dimer for both planar and homeotropic alignments. These parameters
are instrumental in determining the ease of reorientation of the liquid crystal
molecule.
2. Experimental details
The H shaped liquid crystal: bis[5-(4
0
-n-dodecyloxybenzoyloxy)-2-(4
00
-
methylphenylazo)phenyl] adipate, under investigation was synthesized by conden-
sation of 4-methyl-2
0
-hydroxy-4
0
-(4-n-dodecyloxybenzoyloxy) azobenzene with
4-n-dodecylbenzoyl chloride following the procedure reported earlier [10]. The
product was purified by column chromatography (petroleum ether 6080

C: ethyl
acetate, 98 : 2; v/v) over silica gel, and the purity of the compound was performed by
the thin layer chromatography. The compounds were crystallized repeatedly from
ethanol till the constant transition temperatures were obtained. The compound
synthesized was characterized by the combination of elemental analysis and standard
spectroscopic methods. The H shaped liquid crystal dimer (Figure 1a) undergoes
SmC phase at 5148

C on cooling, and crystal to isotropic at 85

C in the heating
phase, which is also clear from the DSC plot of the material shown in Figure 1(b).
The used liquid crystal compound in this study is a dimer, which means that it is
composed of molecules containing the two conventional mesogenic groups linked via
a flexible spacer. This liquid crystal dimer shows quite different behaviour compared
to the conventional liquid crystals. We have used planar as well as homeotropic
alignment for characterisation of this liquid crystal dimer. The study was performed
606 A.K. Misra et al.
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Figure 1. (a) Molecular structure and (b) DSC plot of H shaped liquid crystal dimer: bis[5-(4
0
-
n-dodecyloxy benzoyloxy)-2-(4
00
-methylphenylazo)phenyl] adipate.
Physics and Chemistry of Liquids 607
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by using indium tin oxide (ITO) coated glass plates (sheet resistance is 10 ohmmm
2
and the visible light transmission is more than 90%) having an active area of 25 mm
2
as electrodes. The planar alignment was achieved by treating both the electrodes with
the adhesion promoter and polymer Nylon 6/6 and then rubbing unidirectionally.
For homeotropic alignment, the substrates were simply coated with dilute solution of
lecithin (cetyl trimethyl amonium bromide dissolved in ethyl alcohol) and dried at
200

C for 10 h before characterisation. The complete process of preparation of the

cell has been discussed in earlier papers [13,14]. The macroscopic orientation for both
the alignments was checked by placing sample cell between two-crossed polarisers of
polarising microscope CENSICO 7626. The dielectric response of H shaped liquid
crystal dimer has been studied by using Gain Phase Analyser HP4194A. The
scanning of frequency and acquisition of experimental data has been performed by a
P4 computer, while the temperature was controlled with Instec Hot Plate HCS 302.
The data obtained at higher frequencies were strongly affected by the ITO relaxation,
therefore we have taken measurement upto 10 MHz only [14].
3. Results and discussion
Relative permittivity describes the phase lag between the displacement vector and
applied external electric field in the dispersion region for the sample. The
temperature dependence of the relative permittivity and the dielectric loss of H
shaped liquid crystal dimer are shown in Figures 2 and 3 for both planar and
homeotropically aligned cells. The value of relative permittivity and dielectric loss
40 50 60 70 80 90
14
16
18
20
22
24
26
28
30
32
At Constant Frequency 1000 Hz
For Planar Aligned Cell
For Homeotropic Aligned Cell
Temperature (
0
C )
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a
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i
v
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P
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r
m
i
t
t
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v
i
t
y
Figure 2. Temperature dependence of relative permittivity in planar and homeotropic
alignment for H shaped liquid crystal dimer.
608 A.K. Misra et al.
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increases with increase in temperature for both alignments. For low temperature, the
magnitude of relative permittivity [14] and dielectric loss is small, while it increases
gradually for higher temperatures due to the reorientation of the molecules around
the long axis of the molecules for the planar alignment. The same nature has also
been observed for the homeotropically aligned cell but the magnitude of the relative
permittivity is less as compared to the relative permittivity for the planar aligned cell.
The small difference in the magnitude of the relative permittivity for planar and
homeotropic alignment in the SmC phase indicates that this liquid crystal dimer has
less anisotropic nature in the smectic phase as compared to other conventional
nematic liquid crystal [14].
The anisotropic properties of the liquid crystals are important in determining the
optical response of the liquid crystals [15]. The dielectric anisotropy of liquid crystals
is manifested as a difference in the value of dielectric permittivity measured along the
parallel direction to the long molecular axis c
||
and perpendicular to the long
molecular axis c
?
. The value and the sign of dielectric anisotropy (Dc c
||
c
?
)
depend on the anisotropy in anisotropic distribution of the molecular dipoles in
liquid crystal phases or, more precisely, on the distribution of dipole moments of a
polar group with respect to the long axis of the molecules, i.e. director. The sign of
dielectric anisotropy may be positive or negative, varying from sample to sample.
The substituent dipolar groups will often stabilize the smectic phase but a more
significant consequence of molecular dipoles is through their effect on the molecular
symmetry. Due to this reason dielectric anisotropy has been evaluated and plotted
against temperature and shown in Figure 4. The value of dielectric anisotropy
40 50 60 70 80 90
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8
10
12
14
16
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t
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s
Temperature (
0
C )
For Planar Aligned Cell
For Homeotropic Aligned Cell
Figure 3. Temperature dependence of dielectric loss in planar and homeotropic alignment for
H shaped liquid crystal dimer.
Physics and Chemistry of Liquids 609
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decreases with the increase in the temperature and then sharply reduces to zero at the
isotropic phase transition point. The behaviour of dielectric anisotropy with
temperature for this unusual shaped liquid crystal is found to be the same as
reported for other liquid crystals such as nematic and smectic liquid crystals [9,16].
This H shaped liquid scrystal shows SmC phase from 51 to 48

C on cooling.
The positive value of dielectric anisotropy for this H haped liquid crystal indicates
that molecules are aligned parallel to the applied electric field. After 48

C the phase
transition starts and the value of dielectric anisotropy reduces drastically. At 77

C
the value of dielectric anisotropy reduces to almost zero (0.008), indicating the onset
of isotropic phase and vanishes at almost 75

C and the sample becomes an isotropic

liquid.
Figures 5 and 6 represent frequency dependence of the relative permittivity and
the dielectric loss at a constant temperature of 50

C for planar and homeotropic

aligned cells. It is clear from Figure 5 that there is a peak around 100 Hz for both the
alignments. After this frequency value of relative permittivity is continuously
decreasing upto a particular frequency called critical frequency. Upto this frequency,
the value of relative permittivity for a homeotropic cell is lower as compared to
planar aligned cell, but after this frequency the nature of relative permittivity is
reversed. Due to this, when an electric field is applied to the liquid crystal dimer it
exerts a torque on the director which depends upon the value of dielectric anisotropy.
Due to two types of mechanisms, i.e. reorientation of the director and the presence of
the dielectric torque after SmC phase, one would expect the opposite nature
of relative permittivity after critical frequency. In the dispersion curve shown
in Figure 6, we could see that the relaxation is in the covered frequency range.
40 50 60 70 80 90
0.0
0.5
1.0
1.5
2.0
Temperature (
0
C )
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n
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p
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Figure 4. Temperature variation of dielectric anisotropy for H shaped liquid crystal dimer.
610 A.K. Misra et al.
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100 1000 10000 100000 1000000
12
14
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18
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24
At 50
0
C
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For Planar Aligned Cell
For Homeotropic Aligned Cell
Figure 5. Frequency variation of relative permittivity in planar and homeotropic alignment
for H shaped liquid crystal dimer.
100 1000 10000 100000
0
1
2
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4
5
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7
At 50
0
C
For Planar Aligned Cell
For Homeotropic Aligned Cell
Frequency
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Figure 6. Frequency variation of dielectric loss in planar and homeotropic alignment for H
shaped liquid crystal dimer.
Physics and Chemistry of Liquids 611
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The dispersion behaviour is the same for both the alignments of the sample, but the
magnitude of loss increases for the planar aligned cell in comparison with the
homeotropically aligned cell.
The dielectric data has been analysed using ColeCole equation [8,12,16]. The
low and high frequency deviations in the experimental data have been removed by
adding correction terms in the real and imaginary parts of ColeCole equation as
follows:
c
0
c
0
dc f
n
c
0
1
oc
0
1 2ft
1o
sino,2
1 2ft
21o
22ft
1o
sino,2
1
c
00

odc
c
0
2f
k

oc
0
2ft
1o
coso,2
1 2ft
21o
22ft
1o
sino,2
Af
m
2
where oc
0
is the relaxation strength and c
0
(1) is the high frequency limit of dielectric
permittivity, o is the angular frequency, t is the relaxation time, o is the distribution
parameter, o(dc) is the ionic conductance, c
0
is the free space permittivity, f(o/2)
is the frequency of relaxation and k, n, m are fitting parameters. The term c
0
(dc)/f
n
and o(dc)/ 2c
0
f
k
are added in the above equations for the low frequency effect due
to the electrode polarisation, capacitance and ionic conductance [12,17]. The term
Af
m
is added in Equation (2) for high frequency effect due to the ITO sheet
resistance and lead inductance of the cell. By the least square fitting of
experimental data in the above equation the low and high frequency data have
been corrected [8].
Figure 7 represents the dielectric dispersion of H shaped liquid crystal in terms of
the ColeCole plots for both planar and homeotropically aligned cells. In the figure
the open legend shows experimental data while the solid line represents the best
theoretical fitting of the ColeCole equation into experimental data. We have
evaluated different dielectric parameters such as relaxation strength, distribution
parameter and relaxation frequency from these plots [18]. The relaxation frequency
and relaxation time are related as:
Relaxation time 1,2 Relaxation frequency
Figures 8 and 9 represent temperature variation of the relaxation strength and the
distribution parameter for both the alignments of the present sample. The nature of
the relaxation strength and distribution parameter is the same for both types of
alignments. The value of relaxation strength is higher due to the higher contribution
of the relative permittivity, as discussed earlier for the planar aligned cell as
compared to the homeotropic aligned cell. The value of relaxation strength observed
for the present H shaped liquid crystal dimer is higher after SmC phase, suggesting
that the relaxation observed for the present liquid crystal dimer in the dielectric
spectrum is the combined result of different relaxation mechanisms related to various
molecular motions such as rotational, librational and precessional etc. [19]. The
value of the distribution parameter for the liquid crystal dimer increases gradually
for both planar and homeotropically aligned cells as seen in Figure 9. The high value
of distribution parameter, which describes distribution of relaxation time occurring
612 A.K. Misra et al.
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0
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15 20 25 30 35
0
2
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24
For Homeotropic Aligned Cell
Dielectric Permitivitty
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Dielectric Permitivitty
D
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L
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s
For Planar Aligned Cell
15 20 25 30 35
Figure 7. ColeCole plots in planar and homeotropic alignment for H shaped liquid crystal
dimer, open legends show experimental data while red lines represent best theoretical fit of
ColeCole equation.
40 50 60 70 80 90
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8
10
12
14
16
18
20
22
Temperature (
0
C )
For Planar Aligned Cell
For Homeotropic Aligned Cell
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x
a
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S
t
r
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n
g
t
h
Figure 8. Temperature variation of relaxation strength in planar and homeotropic alignment
for H shaped liquid crystal dimer.
Physics and Chemistry of Liquids 613
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into dielectric equation suggests that the H shaped liquid crystal dimer follows the
ColeCole theory.
Another important dielectric parameter, the relaxation frequency, is plotted
against temperature as shown in Figure 10 for both types of aligned cells of the liquid
crystal dimer. The nature of relaxation frequency is the same for both the alignments,
but the magnitude of relaxation frequency is shifted towards the higher side for the
homeotropic aligned cell. The reason for this increment is the flexibility of the long
molecular chain, which causes mutual correlation in the orientation of molecules
giving rise to a relative weak component of induced dipole moments [20,21] having
j
H
4j
P
(here j represents a component of induced dipole moment and suffixes H
and P represent homeotropic and planar alignments respectively). This difference in
the component of the induced dipole moment is due to the reason that the time
necessary for orientation of the molecule in the presence of a field is longer than the
time required for changes of chain conformation. This means that the dimeric
molecules rotate in field but their behaviour is determined by the mesogenic part as a
whole, not as molecules. The molecular length is relatively long for the present liquid
crystal dimer so that the necessary time for their orientation in the electric field is
longer than the time required for changes in chain conformation, and therefore, the
value of relaxation frequency is small in the SmC phase. In the SmC phase, the
dielectric spectrum of the liquid crystal dimer shows only one type of relaxation
around a few kHz of frequency; after the SmC phase the relaxation frequency
increases due to the presence of other relaxation mechanisms near the isotropic phase
transition point [19].
40 50 60 70 80 90
0.20
0.25
0.30
0.35
0.40
For Planar Aligned Cell
For Homeotropic Aligned Cell
D
i
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t
r
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b
u
t
i
o
n

P
a
r
a
m
e
t
e
r
Temperature (
0
C )
Figure 9. Temperature variation of distribution parameter in planar and homeotropic
alignment for H shaped liquid crystal dimer.
614 A.K. Misra et al.
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4. Conclusion
We have investigated the dielectric relaxation of a H shaped liquid crystal having azo
central linkage inside the dimer. We have observed one relaxation process in the
SmC phase, and the relaxation frequency is shifted towards the higher side for
the homeotropically aligned cell as compared to the planar aligned cell due to the
flexibility of the molecular chain. After a particular frequency, the nature of relative
permittivity is reversed for both types of alignments. This is due to the presence of
two types of mechanisms, i.e. reorientation of the director and existence of the
dielectric torque due to applied electric field. Therefore, one would expect an
opposite nature of relative permittivity after critical frequency. The higher value of
relaxation strength suggests that the relaxation mechanism is a combined result of
various molecular motions for a planar aligned cell. The relaxation phenomenon for
this unusual shaped liquid crystal is explained by ColeCole study, the relaxation
frequency is almost temperature independent. But near the isotropic phase transition
temperature it increases considerably because at this transition other
various molecular motions such as rotational, librational and precessional starts
dominating.
Acknowledgements
One of the authors (AKM) is thankful to UGC, New Delhi for the II year grant of Dr. D.S.
Kothari Post Doctoral Fellowship No. F.4.2/2006 (BSR)-13-234/2008(BSR).
40 50 60 70 80 90
500
1000
1500
2000
2500
Temperature (
0
C )
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a
x
t
i
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n

F
r
e
q
u
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n
c
y

(
H
z
)
For Planar Aligned Cell
For Homeotropic Aligned Cell
Figure 10. Temperature variation of relaxation frequency in planar and homeotropic
alignment for H shaped liquid crystal dimer.
Physics and Chemistry of Liquids 615
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