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Submitted on 1 Jan 1988

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Zigzag disclinations in uniaxial nematic liquid crystals

Yves Galerne, Jacques Itoua, Lionel Liébert

To cite this version:

Yves Galerne, Jacques Itoua, Lionel Liébert. Zigzag disclinations in uniaxial nematic liquid crystals.

Journal de Physique, 1988, 49 (4), pp.681-687. �10.1051/jphys:01988004904068100�. �jpa-00210743�

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Zigzag disclinations in uniaxial nematic liquid crystals

Yves Galerne, Jacques Itoua and Lionel Liébert

Laboratoire de Physique des Solides, Bât. 510, Université de Paris-Sud, 91405 Orsay Cedex, France (Requ le 23 octobre 1987, accepté le 17 dgcembre 1987)

Résumé.

2014

Des lignes de disinclinaison en zigzags ont été observées dans des cristaux liquides nématiques

uniaxes (4-méthoxy-benzylidène-4’-n-butylaniline et 4-n-décyloxy benzoate de 4’n-hexyloxy phényl) qui

ressemblent beaucoup aux lignes zigzags déjà étudiées dans les nématiques biaxes. Elles sont cependant produites par un mécanisme différent. Il en résulte que les variations de l’angle des zigzags de disinclinaisons

en fonction de la température, sont différentes dans les nématiques uniaxes et dans les nématiques biaxes. On

en déduit un critère assez simple de biaxialité des phases nématiques.

Abstract.

2014

Zigzagging disclination lines have been observed in uniaxial nematics (4-methoxybenzylidene-4’- n-butylaniline and n-hexyloxy-4’ phenyl n-decyloxy-4 benzoate), which very much resemble the zigzags already

studied in the biaxial nematics. They, however, originate from a different mechanism. It results a different temperature behaviour of the angle of the disclination zigzags in the uniaxial and the biaxial nematics, which

leads to a rather simple criterion for the biaxiality of the nematic phases.

Classification Physics Abstracts

61.30

-

61.70G

-

61.70J

1. Introduction.

Recently, 1 -disclinations have been observed in 2

biaxial nematic liquid crystals [1]. They are lines along which the local biaxial order is broken and reduced to the uniaxial order. The disclination lines in the biaxial nematics bear therefore a director, parallel to them for symmetry reasons, which in-

teracts with the anisotropic elastic field of the

surrounding liquid crystal. This interaction makes the disclination lines to orient along preferred direc-

tions and to keep the shape of zigzags. Because this mechanism needs two directors (one to be broken on

the line, and the other to realize the couplings of the

line with the bulk), it has reciprocally been suggested

that the zigzagging disclination lines are a character- istic feature of the biaxial nematics, and that their observation could indicate biaxiality in the nematic

liquid crystals [2].

In the paper we show that zigzagging disclination lines can also exist in the uniaxial nematics, with a slightly different mechanism. Contrarily to what we

believed earlier, their observation is therefore not an

absolute criterion of biaxiality [3]. Other features,

such as the temperature variations of the angle of the zigzags, must be considered as well to ascertain

biaxiality.

2. Experimental method.

The experimental part of this work is performed on thermotropic uniaxial nematics [4] : the well-known

4-methoxybenzylidene-4’-n-butylaniline (MBBA),

and n-hexyloxy-4’ phenyl n-decyloxy-4 benzoate (HPDB), in the temperature ranges : 22 °C to 47 °C and 80 °C to 86 °C, respectively. The experimental procedure is the following. The nematic compound

is inserted between two parallel glass plates treated

with silane in order to favor the homeotropic orien- tation, and separated with mylar spacers of known thickness. The sample is placed inside a Mettler

stage to regulate its temperature, and observed under a polarizing microscope. Applying a gentle

pressure on the cover slide of the sample makes the

nematic liquid crystal flow, and reorient in the shear flow thus created. This effect, known for a long time, results from the negative sign of the Leslie

viscosity coefficient a 3; it exists in most of the available nematic liquid crystals, including MBBA [5]. In this manner, it is possible to put a whole domain of the sample in planar orientation (as can

be tested by rotating the stage of the polarizing microscope) while the rest remains homeotropic (Fig. g ) 1). A disclination line of 1 -strength 2 is thus

created at the boundaries between domains of

Article published online by EDP Sciences and available at http://dx.doi.org/10.1051/jphys:01988004904068100

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682

Fig. 1.

-

Cut of a homeotropic sample submitted to local

flow (arrow). A planar domain surrounded by a discli-

nation loop (hatched dots) appears. The lines sketch the orientations of the nematic director.

different orientations. (Disclination lines of higher

orders which appear as thicker lines under the

microscope, are also obtained in this way, but we do not consider them here.) In fact, the planar orien-

tation is produced in the bulk of the sample only. On

the glass surfaces, the nematic director is tilted because of the weak homeotropic anchoring. Be-

tween these two orientations in the vicinity of the glass surfaces, the orientation is distorted. Because the configuration of figure 1 is not strongly anchored,

it slowly relaxes, making the disclination lines mi- grate, and after a long time disappear. The whole sample has then recovered its equilibrium with the complete homeotropic orientation. Before this oc-

curs, however, we have the opportunity to study the

behaviour of disclination lines under quasi-steady

conditions.

3. Transformation of the wedge to the twist discli- nation.

3.1 WEDGE-DISCLINATION LINE. - We restrict our

attention now to the symmetric cases where the 1 -disclination lines, which separate two domains of

2

different orientations, are perpendicular to the plane

of both the planar and homeotropic orientations, and located at equal distances from the plates. In the simplest view, the molecules are arranged around

the so-called wedge-disclination lines of positive (Fig. 2) or of negative sign. (Both cases are equival-

ent within our approximations (see below) ; we

therefore explicitly consider the + 1 2 -wedge-discli-

nation lines only.) These configurations do not

involve the twist elastic deformation. Making the approximation of twist anisotropy only (Kl

=

K3

=

K =F K2) is therefore equivalent to making the one-

constant approximation in these specific cases. The

free energy per unit length of the wedge-disclination

line is therefore expressed [6] as

where D is the sample thickness, a is the diameter of the core of the wedge-disclination - 100 A, Fc is the

Fig. 2.

-

Wedge-disclination line of + 1-strength. To

simplify, the details of the anchoring near the plates are

not represented. The hatched dot schemes the core of the line.

energy per unit length of this core, estimated [6]

-

K/2, and FS is the surface energy per unit length

of the disclination line, due to the planar orientation in the left part of the sample. This Fs term includes

the anchoring energy, which results from the tilting

of the director onto the glass surfaces, and the elastic

energy of the distorsion in the vicinity of the

surfaces. Fs results in a transverse force which drives the line to the left boundary of the sample until the perfect homeotropic orientation is restored.

3.2 TWIST-DISCLINATION LINE. - In the uniaxial nematics, all the 1 2 -disclination lines can topologi- cally transform from one type to another one, i.e.

they all belong to the same homotopy class [7]. The wedge-disclination described in figure 2 can thus continuously transform into a twist-disclination, at

least in its close vicinity as sketched in figure 3. In fact, this transformation really occurs if the free

energy involved in the new orientation (Fig. 3) is

lower than the previous one (Fig. 2). This leads one to estimate FT, the free energy of the new orientation per unit length along the z-axis, in order to compare it to FW. FT is the addition of the surface energy

Fs, due to the planar orientation as before, to the

bulk elastic energy of the new distortion (Fig. 3).

This distortion is the superposition of two simpler

deformations : (I) a planar twist deformation which rotates the molecules parallel to the yz-plane around

the twist disclination line, and (II) a bend defor- mation in the left part of the sample which rotates

the molecules about the y-axis from parallel to the xy-plane to parallel to the yz-plane. The planar twist

deformation (I) is a twist of wave vector parallel to

the x-axis superposed to a splay, while the defor- mation (II) consists of a bend superposed to a twist

of wave vector parallel to the y-axis. Both defor- mations (I) and (II) are therefore orthogonal and

have additive elastic energies. Let us now estimate

these respective elastic energies with the assumption

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Fig. 3.

-

Twist-disclination line with the conventional

representation of the nematic directors as nails. The hatched parts scheme the core of the line. a) Cut along the xy-plane. b) Cut along the xz-plane. The dashed line represents the equilibrium direction of the line. The arrow

indicates the positive sense of orientation of the angles.

of twist anisotropy only Kl

=

K3

=

K =f:: K2. The

free energy of the planar twist deformation (I) per unit length along the z-axis is given from a calculation

by Ranganath [8] :

The calculation of deformation (II) has to be done separately. The deformation (II) is specified by the angle 0 (x, y ) of the rotation around the y-axis that it

exerts on the molecules. e (x, y ) is thus solution of the Euler-Lagrange equation:

with the boundary conditions :

and 0 (x = 0, y = 0 ) = Ir - For the sake of simplici-

2

ty, it is useful to complement the boundary con-

ditions in the yz-plane. We can thus assume that 0 (x

=

0, y) varies linearly between its two limits 0

and 7r , respectively at y

=

± D and y

=

0. The

2 p y 2

Fourier analysis of this problem is then simple. It

shows that, for x 0 :

the deformation (II) is therefore :

Limiting this series to its first term, we deduce the

expression of the free energy per unit length of the

twist-disclination line to be :

where Fc, the energy per unit length of the core of

the twist-disclination, may be estimated - KK2/2.

3.3 MECHANICAL TRANSITION OF THE WEDGE TO THE TWIST-DISCLINATION. - As discussed above, the topological transformation of the + § or - § -

2 2

wedge-disclination into a twist-disclination spon-

taneously occurs if the energy balance FT FW is satisfied, i.e. for :

This inequality shows that the wedge to twist

transformation appears for sample thicknesses D above some threshold value Do. Considering the published values of the elastic constants of MBBA

[9] and of other compounds [10] (which show that

K2 - 2), Do may be evaluated to be of the order of

K2

1 )JLm. This makes the transformation easily observ-

able in the usual samples. Let us also notice that above the threshold of the external forces produced by the glass surfaces of the sample, the system loses

one symmetry element, that is the xy-mirror of symmetry (see for instance Fig.3b). Such a symmetry breaking above threshold typically indicates that the

wedge-twist transformation of disclinations is a

mechanical instability or a mechanical transition.

4. Tilting of the twist-disclination line.

The destruction of the xy-mirror of symmetry at the wedge-twist transition of the disclination (Sect. 3.3)

allows the disclination line to tilt by an angle 00 (dashed line in Fig. 3b), and it actually tilts

because of its elastic couplings to the surfaces through the term F2. In order to calculate the tilt

angle 00, let us estimate the energy of the tilted disclination line per unit length of the z-axis. Keeping

the line located at the same position, the surface of the left part of the sample, and therefore the

anchoring energy Fs, remain the same as in sec-

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684

tion 3. Consequently, Fs does not depend on 0 0. Because of the tilt, the length of the line

corresponding to the unit length on the z-axis is e2

multiplied by a factor of 1 + 2 ) as therefore the

B 2 /

first and third terms of equation (6) which become

term of equation (6) can be calculated as in sec-

tion 3.2, just considering the amplitude change

(-f - 0 0 instead of2 ) of the bend deformation (II)

due to the tilting of the line. It becomes

16 ( 7T 00 ) 2 J- The complete expression of 7T 2 00 KK2. The complete expression of

the twist-disclination energy per unit length of the z-

axis is therefore :

The tilt angle of the disclination line at equilibrium is

then deduced to be :

N - / N - I

Though the disclination line is tilted, if referred to the initial orientation of the sample, it has to

maintain its general direction, along the z-axis. The way for the line to satisfy this apparent paradox, is clearly to make zigzags as in the biaxial nematics [1].

The orientation of the director around the « zag »

(the segment of line tilted by - 00) is deduced from the orientation around the « zig » (Fig. 3) by an xy- mirror of symmetry. This indicates that the corre-

sponding twist-disclinations have opposite signs in

the « zigs » and the « zags ». Let us notice that the twist-disclinations discussed here originate from the

+ 1 2 -wedge-disclination of figure 2. Of course, simi-

lar results are obtained when starting from a

1 -wedge-disclination, 2 g but with changed signs for

the twist-disclinations of the «zigs» and the

« zags », compared to their signs in the + 1-wedge-

disclination case.

5. Experimental results.

5.1 GENERAL OBSERVATION. - Zigzagging discli-

nation lines have been obtained following the exper-

imental procedure described above, in the whole temperature range of the nematic phases of MBBA

and HPDM, and for sample thicknesses varying

from a few microns to 100 f-Lm (Fig. 4). Except when hung to a dust grain, the lines are slowly moving due

to the relaxation of the planar anchoring. The

observation of this drift is important to make sure

that the lines are freely suspended in the bulk, and

not erratically stuck on the glass surfaces. The

velocity of this displacement is however very slow

( ~ 10 f-Lm/s), and does not modify the equilibrium shape of the line as is exp,erimentally verified when

the line stops for a while (e.g. hindered by some dust aside). The samples are observed between crossed

polarizers oriented parallel to the sides of the

photographs. In figure 4a, the sample is placed so

that the planar region is extinguished, which means

that the planar direction is oriented perpendicular (or parallel) to the polarizers. In figures 4b and 4c,

the sample is tilted from this original orientation. As

a result, the planar domain lightens and a black fringe appears along the disclination line. In all the cases, the general direction of the disclination lines,

or more exactly, the external bisectors of the zigzags,

are perpendicular to the planar direction revealed by

the polarizers, in accordance with the above dis- cussion (end of Sect. 4).

5.2 BLACK FRINGES.

-

As denoted above, the disclination line appears as decorated with black

fringes when the sample is slightly rotated from its

extinguished position (between crossed polarizers).

More specifically, the fringes follow the « zigs » for a positive rotation (photo 4b), and follow the « zags » for a negative rotation of the sample (photo 4c).

This is an optical effect due to birefringence. The fringes (which in principle are grey and not black)

reveal the places where the average direction of the molecules is oriented along the polarizers. The

measurements of the abscissa x’(= - x ) of the fringe

referred to the disclination line as a function of the

angle 0 of rotation of the sample are given in figure 5

for a sample of thickness D

=

45 tLm. 0 (x’ ) appears thus to vanish exponentially with a characteristic

length 6 - D.

This result is to be compared with the average value of 0 over the sample thickness. Restricting the

calculations to first order, we find from equation (4) :

This expression is rather consistent with the exper- imental results of figure 5, if one takes into account

that : 2 - ; . It therefore yields a direct support to

7T 4

the model of the bend distortion in the planar region, with the molecules arriving tangent to the

twist-disclination line (Fig. 3b). However, one may notice that the experimental and the calculated

characteristic lengths differ by a factor of about 2.

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Fig. 5.

-

Rotation angle ø of the sample versus the

abscissa x’(= - x) of the black fringe, in a sample of

thickness D

=

45 Rm.

This significant departure from the model could indicate that the planar orientation of the sample is

not so strongly held at the glass surfaces as supposed

in section 3.

5.3 ZIGZAG ANGLES.

-

The angles of the zigzagging

disclination lines present large variations from one to another. Such variations could originate from

hazardous surface perturbations unsufficiently con-

trolled by the too weak planar alignment of our samples (as already suspected above to explain the

increased values of g). These variations being erratic,

it is possible to filter them statistically. We thus used

video recordings to make data accumulations (up to

30-50 in each case). These experimental means are

also very convenient to select zigzags at equilibrium

and to take series of pictures of the same zigzag for

different rotation angles of the microscope stage to

measure the black fringe (Sect. 5.2).

The zigzag angles have been measured far from the peaks to avoid the distortions around it [11], and

under different conditions of temperature and

sample thickness for both the MBBA and the HPDB compounds (we used then a cleaner source than for

Fig. 4.

-

Photomicrographs of zigzagging disclination lines between crossed polarizers, oriented horizontally and vertically. The homeotropic and planar parts of the samples are respectively on the right and on the left sides of the photos. The photos are taken with the same

magnification. The distance of the black fringe to the

disclination line is typically of the order of the sample

thickness. a) 10 lim-thick sample of HPDM at 85 °C,

oriented perpendicular to the polarizer. b) 45 JLm-thick sample of MBBA at 35 °C, rotated by a small positive angle (following the sense of the arrow in Fig. 3b) referred

to the direction of the polarizer. c) 90 tlm-thick sample of

HPDM at 81 °C rotated by a small negative angle.

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686

the photos). No dependence of the zigzag angles on

the temperature, nor on the compound has been

observed. This observation is clearly consistent with

equation (9). However, one may notice that our

calculations are based on the approximation Kl

=

K3, which experimentally is rarely verified (e.g. in

MBBA [9], K3/ Kl -- 1.5). An exact calculation, releasing this approximation, would express the tilt

angle 0 0 of the disclination line as a function of the ratios of the three elastic constants Kl, K2 and K3. Through them, 00 would in fact slightly depend

on the nature of the compounds, and on the temperature. These variations should however re-

main negligible if compared to 00 itself.

The only variation of the zigzag angle 00 that we

have found is a regular increase with the sample

thickness D. Figure 6 shows the measurements of

1/00 versus In (Dla) for MBBA (corresponding to

D ranging between 5 to 100 Rm), together with the

calculated variations from equation (9) (straight line). The agreement between the experimental and

the calculated variations is correct within the stan-

dard deviations of the data (represented as bars).

The curvature in the variations of the experimental

data that one could notice in figure 6 is probably not significant. It could however be due to higher order

terms that we have neglected in the calculations (e.g.

in Eqs. (1) and (2)).

Fig. 6. - Inverse tilt angle 1/80 of the disclination line

versus In (D/a ). The experimental data are represented

with their standard deviations (500/00-3-4%, and

BD - few microns). The straight line corresponds to the

calculated variations from equation (9).

6. Discussions.

The zigzagging disclination lines, reported here in

the uniaxial nematics, resemble those already ob-

served in the biaxial ones [1]. We may however try

to find differences which could be used as criteria for the biaxiality. A difference that one can first notice,

is the black fringe discussed here in details, and unobserved in the biaxial nematic phase [1]. In fact,

as discussed in section 5.2, this black fringe is

relevant to the value of g, which is determined by the experiment, and not to the uniaxial or biaxial nature of the liquid crystal. In reference [1], the sample was

oriented with a magnetic field H which imposed a small g. As a result, the black fringe was stuck to the

disclination line, and thus not observable. The observation (or non-observation) of the black fringe along a zigzagging disclination line is therefore not related to uniaxiality (or biaxiality).

A difference between uniaxial and biaxial nematics is the temperature variations of the angles of the

disclination zigzags. In the biaxial nematics, 00 strongly depends on temperature, because it is

directly proportional to the biaxial order parameter [1]. In the uniaxial nematics as discussed in section 5.3, 00 is independent of, or slightly dependent on

temperature. This suggests to use the temperature

variations of the zigzags as an indication of biaxiality [3]. Such measurements could be an easier task than

succeeding an undoubtless conoscopic figure [12]

(which needs a perfectly oriented sample).

As discussed in section 5.3, we suspect that the

large uncertainties of our measurements arise from the too weak planar alignment of our samples. It

would thus be useful to improve the planar orien-

tation by applying a horizontal magnetic field on the sample. The expression of 00 would then be modified

by essentially replacing D/2 in equation 9 b the magnetic correlation length g H

=

K XaH [6]

(which becomes the pertinent length of the prob- lem).

Applying a magnetic field onto the sample would

also be interesting to observe the continuous trans- formation of the disclination lines. When the magne- tic field is increased up to a few kiloGauss, ç H is decreased to a few microns (since KIYA -

5 dynes), pushing the black fringe close to the

disclination line. The black fringe would then disap-

pear, making the zigzag resemble very much the one observed in the biaxial nematics. The decrease of

6H would also produce an increase of the zigzag angle 00 until the mechanical transformation of the twist to the wedge-disclination line occurs (Sect. 3.3). At the threshold value H - 150 kG

(from Eq. (7), replacing D/2 by gH)’ the line straightens, i.e. 00 jumps from its maximum value

( = 23° from Eq. (9)) to zero. The twist to wedge-

disclination transformation is therefore a first-order mechanical transition. It is worth noticing that such

an experiment could probably be more easily per-

formed using lyotropic nematic liquid crystals doped

(8)

[13].

In conclusion, we have observed disclination lines in the form of zigzags in the uniaxial nematics, which resemble very much the zigzags already observed in the biaxial nematics. The zigzagging disclinations in the uniaxial nematics, however, are produced by a

different mechanism than in the biaxial nematics.

They result from the elastic interaction between two

conflictual orientations of the director far from the

disclination line and in its immediate vicinity, and not strictly on it as in the biaxial nematics. (This is impossible for the disclinations in the uniaxial nema-

tics because they have an isotropic core, and thus

director, i.e. typically in the uniaxial nematics. Let

us notice that other conflictual configurations than

that studied here, could similarly produce zigzagging

disclination lines in the uniaxial nematics. For in- stance, a wedge-disclination (provided that it is

properly stabilized) could also make zigzags if pro- duced in a planar sample and oriented parallel to this planar alignment.

It is a pleasure to thank Drs. G. Durand, Ph.

Martinot-Lagarde and P. Pieranski for very helpful discussions, and Dr. C. Germain for providing us

with MBBA and HPDB.

References

[1] GALERNE, Y. and LIÉBERT, L., Phys. Rev. Lett. 55 (1985) 2449.

[2] MALTHÊTE, J., LIÉBERT, L., LEVELUT, A. M. and GALERNE, Y., C. R. Acad. Sci. 303 (1986) 1073.

[3] GALERNE, Y., Colloque d’expression française sur

les Cristaux Liquides (Arcachon), septembre

1987 (to be published).

[4] Similar studies in lyotropic uniaxial nematics are

independently developped by M. Mihailovic and M. Kléman (to be published).

[5] GÄHWILLER, C., Phys. Rev. Lett. 28 (1972) 1554.

[6] DE GENNES, P. G., The Physics of Liquid Crystals (Clarendon, Oxford) 1974.

[7] MERMIN, N. D., Rev. Mod. Phys. 51 (1979) 591.

[8] RANGANATH, G. S., Mol. Cryst. Liq. Cryst. 87 (1982) 187.

[9] DE JEU, W. H., CLAASSEN, W. A. P. and SPRUIJT,

A. M. J., Mol. Cryst. Liq. Cryst. 37 (1976) 269.

[10] DE JEU, W. H. and CLAASSEN, W. A. P., J. Chem.

Phys. 67 (1977) 3705.

SCHAD, H. and OSMAN, M. A., J. Chem. Phys. 75 (1981) 880.

[11] GALERNE, Y., to be published.

[12] GALERNE, Y., ISAERT, N., LEVELUT, A. M., LIÉ-

BERT, L. and MALTHÊTE, J., Colloque d’expres-

sion française sur les Cristaux Liquides (Arca- chon), septembre 1987 (to be published).

[13] KROIN, T. and FIGUEIREDO NETO, A. M., Phys.

Rev. A 36 (1987) 2987.

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