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Theory of flow alignment in biaxial nematics and nematic discotics

H. Brand, H. Pleiner

To cite this version:

H. Brand, H. Pleiner. Theory of flow alignment in biaxial nematics and nematic discotics. Journal de

Physique, 1982, 43 (6), pp.853-858. �10.1051/jphys:01982004306085300�. �jpa-00209462�

(2)

Theory of flow alignment in biaxial nematics and nematic discotics

H. Brand (*) and H. Pleiner

FB 7, Universität Essen, D-4300 Essen, W.-Germany (Reçu le 21 janvier 1982, accepté le 16 fevrier 1982)

Résumé.

2014

Nous présentons une théorie microscopique de l’orientation des cristaux liquides nématiques (et nématiques discotiques) biaxes dans une expérience d’écoulement. Nous proposons trois configurations géomé- triques très simples pour mesurer les trois paramètres réversibles qui sont affectés. Le cas particulier des nématiques discotiques uniaxes est discuté séparément. En outre, nous discutons d’effets similaires dans les smectiques C et cholesteriques.

Abstract

2014

We present a microscopic theory for the flow alignment in biaxial nematics and nematic discotics and we propose three simple geometrical configurations to measure the three reversible parameters involved.

The uniaxial special case for nematic discotics is discussed separately. In addition we discuss similar effects in smectics C and cholesterics.

Classification

Physics Abstracts

.

61.30

-

03.40G - 47.90

1. Introduction.

-

The interest in the theoretical

description of biaxial nematics increased considera-

bly since the first (lyotropic) biaxial nematic liquid crystal has been produced last year [1]. In the present letter we will discuss in some detail one aspect of the

hydrodynamic description [2-5] of biaxial nematics

(and nematic discotics) namely the flow alignment

under an external shear flow. This experimental arran-

gement is well known for uniaxial nematics [6] and

serves there (via determination of the alignment angle) to determine the only nontrivial (i.e. different

from 1 or 1/2) reversible transport parameter of uniaxial nematics. On the other hand this coefficient

can be calculated by means of Poisson brackets [7].

In section 2 we will carry out the same procedure for

biaxial nematics (and nematic discotics) and, as it

turns out, the three reversible transport parameters

can be determined separately by the study of three simple geometric orientations of the preferred direc-

tions n and m of biaxial nematics. These coefficients

(at least the instantaneous parts of them) are expressed by the four microscopic « order parameters >> which

are necessary for a consistent description of the sys- tem [8, 9]. Of course, the uniaxial situation is always

contained as a special case in our presentation. In

section 4 we will discuss separately the flow alignment

in uniaxial nematic discotics exploiting previous work

by D. Forster [7] on the usual (rod-like) type of uniaxial nematics. Discotic liquid crystals have been produced

for the first time in 1977 by S. Chandrasekhar et al. [10]

and since then columnar phases of hexagonal and rectangular symmetry as well as nematic like and cholesteric like discotic liquid crystals have been produced [11-15]. In section 5 we briefly investigate

a shear flow experiment which can be used to deter-

mine one of the two reversible parameters which enter the reversible currents [16, 17] of smectics C and we

clarify the microscopic nature of the variable charac-

terizing the spontaneously broken rotational symme- try in smectics C. In addition we calculate in section 6 the instantaneous part of the coefficients gkl entering

the hydrodynamic description of cholesterics. These terms, which couple the displacement field to the symmetrized gradients of the velocity field, have been

introduced by the authors recently [17].

2. Flow alignment in biaxial nematics.

-

The non-

linear hydrodynamic equations for biaxial nematics have been derived for the first time by the present authors very recently in detail [2]. As has been pointed

out, there, the reversible currents for the three variables

characterizing the spontaneously broken rotational symmetry in real space take the form

Article published online by EDP Sciences and available at http://dx.doi.org/10.1051/jphys:01982004306085300

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854

with

In the following we only need equations (2.1)

and (2.2). For the other reversible currents as well

as for the irreversible and static contributions we refer to reference [2]. As it turns out it proves to be conve-

nient to introduce Eulerian angles to characterize the flow alignment angles. Using standard notation of textbooks on mechanics we have

We consider in the following a stationary shear flow,

which we can assume without loss of generality to lie

in the y - z plane (i. e. VyVz # 0). Using (2 .1 )-(2 . 5)

we then find for al, Ct.2 and as (in order to guarantee

stationarity)

Since the general expressions (2.6)-(2.8) are not

very illuminating we discuss three simple geometries :

where the equations for a2 and as are satisfied identi-

cally.

-

The geometrical picture corresponding to case (i) has been plotted in figure 1.

(ii) (p = 0 = 00 :

The equations for al and as are again satisfied identi-

cally and we get the situation shown graphically on figure 2.

Fig. 1.

-

Flow alignment angle 0, which measures the

coefficient al (2.9); the preferred direction n lies in the shear plane, while m is orthogonal to it.

The direction m is orthogonal to the shear plane

and the vector n is titled by the angle 0, which is determined by the coefficient al (2. 9).

Fig. 2.

-

Flow alignment angle 9 which measures the

coefficient a2 (2. 10) ; both preferred directions, n and m,

lie in the shear plane.

As is immediately seen from figure 2 both preferred

directions m and n lie in the shear plane and the corresponding alignment angle 0 is determined by the

coefficient a2 (2. 10).

In the third case the equations for al and a2 are

satisfied identically whereas a5 is determined by

(4)

The corresponding geometrical situation is plotted

in figure 3.

Fig. 3.

-

Flow alignment angle T which measures the coefficient as (2.11); the preferred direction m lies in the shear plane, while n is orthogonal to it.

In the third case n points out of the shear plane and,

m is oriented in the plane according to (2 .11 ).

On the other hand, it is possible by measuring the alignment angles in the three different geometries

to obtain measured values of the reversible transport parameters ai, a2 and a5 by means of equations (2. 9)- (2 .11 ).

3. Microscopic description.

-

In the next step we relate the transport parameters al, a2 and as to the

microscopic order parameters using a technique which

is quite similar to that proposed for uniaxial nematics

by D. Forster [7]. The hydrodynamic variables cha-

racterizing the broken rotational symmetry can be expressed by the elements of the quadrupole tensor Rij in the following way (n°/%Z == ê3, mO/êy- == ê2)

where Qij = Rij > and where Rij is the operator for

the quadrupole tensor [7]. Using these definitions for the variables bni, 6m; we have the commutation relations (or rather Poisson brackets) with the opera- tor for the angular momentum L

Generally, the coefficients cxl, Ct.2 and a 5 contain two contributions : an instantaneous one arising

from the frequency matrix and a collision dominated one, which arises from the non-hermitian part of the

memory matrix [7, 18]. Then we find for the instan- taneous contributions to the coefficients «1, a2 and as

where g is the linear momentum density and Q is the

sum of the moments of inertia Ii.

As for uniaxial nematics [7] the non-instantaneous collision-dominated contributions to al, a2 and a5

are expected to be very small. In a last step we connect the quantities Qij to the four microscopic order parameters (S, A, q, and il’) which are necessary to guarantee an appropriate microscopic description

of biaxial nematics [8, 9].

Using the work of R. G. Priest and T. C. Lubensky

we have in detail

with

Taking into account the relation [7]

/

we have B ’e

(5)

856

Combining equations (3.3)-(3.6) we obtain the final result (expressing the phenomenological coeffi-

cients al, a2 and a5 by the microscopic order para- meters S, L1, r¡ and r¡’)

with

Thus we have outlined in this section on biaxial nema-

tics (or nematic discotics) a possibility to get from flow alignment experiments informations about the

microscopic order parameters and vice versa.

4. Flow alignment in uniaxial nematic discotics.

-

Recently nematic discotics have been synthesized

and flow alignment measurements are possible [19].

It is the purpose of the present section to show that the theory of flow alignment for uniaxial nematic discotics is implicitly contained in the previous cal-

culations of D. Forster for uniaxial rod-like nematics

[7]. Furthermore, we discuss an experimental scheme appropriate for uniaxial nematic discotics. For the

flow-alignment angle D. Forster derived the result

with

This expression is also contained in our general for-

mulas (3. 7) and (2 . 9)-(2 .11 ), if, there, the biaxia-

lity is switched off, i.e. al

=

a2 = - 2 A, as = 0,

L1 = q = 11’ = 0.

For extreme rod-like molecules (1 - 0)

À

=

3 S/(2 + S) and the flow alignment angle 0

varies between 7r/4 (for S

=

0, no ordering) and zero (for S

=

1, full ordering), In the case of extreme disc- shaped molecules (I, --+ 0) one obtains A

= -

3 S/(4 - S)

and the flow-alignment angle varies between 7r/4 (for S

=

0) and 7r/2 (for S

=

1). Thus, for discotics

the flow-alignment angle increases for increasing ordering in contrast to (rod-like) nematics. Of course, for full ordering S

=

1 the molecules are horizontal,

i.e. 0

=

900 for discotics and 0

=

00 for (rod-like)

nematics (cf Fig. 4). The results for S

=

1 (e.g. À = - 1

for extreme discotics) were previously given by

Fig. 4a.

-

Flow alignment angle for rod-like molecules

(IIi It N 5, S z 0.8).

Fig. 4b.

-

Flow alignment angle for disc-shaped molecules (It/ II N 5, S = 0.8).

Volovik [20]. However, S

=

1 is never reached in

nature. In figure 4 we sketch the experimental situa-

tion for realistic values of S.

5. Flow alignment in smectics C.

-

As is well known [6, 16] smectics C has two variables charac-

terizing spontaneously broken continuous symme- tries : one characterizing the broken translational symmetry along the layer normal (called 3-axis in the

>

following) of the smectic layers (like in smectics A)

and one characterizing a rotational symmetry about this 3-axis.

If the molecules are assumed to lie in the 1-3 plane

in equilibrium, the rotational degree of freedom is described by fluctuations of n which are perpendicu-

lar to the 1-3 plane. The reversible part of the dynamic

equation for that variable reads [16, 17.]

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(In reference [17] the coefficients )t(1), A(3) are called

-

2 a2, - 2 al, respectively,)

By inspection of equation (5.1) it becomes obvious

immediately that a stationary flow alignment experi-

ment is possible only for V 1 V 2 =1= 0 or V 2 V 1 =1= 0;

thus only )t(3) (but not )t(1») is measurable by means

of a flow alignment angle 0, and we find

In order to relate ;}1) and A(3) to the microscopic

order parameters one must first express the hydro- dynamic variable bn2 in terms of the operators Rij.

Thereby one has to take care of the fact that

( Rij > _-- Qij is not diagonal in smectics C [6].

Using the relation

one finds that

(with ç

=

Q13(Q22 - Q33)-1) is the appropriate expression because it leads to the canonic commu-

tation relation

The existence of Q13 =A 0 is characteristic for smec-

tics C (compared to nematics or smectics A).

Using (5.4) we find for the instantaneous parts of A (1) and A(3) the relations

and

Thus it becomes possible to give a connection between the flow alignment parameter  (3), which is acces-

sible to experiment, and the quantities Qij (espe- cially Q13 !) which can be calculated by fully micro- scopic theories.

6. Remark on a reversible parameter in choleste-

rics.

-

Recently the present authors have shown [17]

that in the hydrodynamic equation for the variable Ri characterizing the broken symmetry of cholesterics, symmetry arguments allow for two reversible trans-

port coefficients gi and g2 which were not taken into account previously [16, 21], i.e.

(p - pitch axis; 2 trio

=

pitch).

Although the phenomenological parameters g 1 and g2 are not measurable by flow alignment experiments [22], they show some similarities with the reversible transport parameters in nematics and smectics C described above. We will derive a microscopic expres- sion for gl and g2 in the same spirit as we have done

above for the A’s and a’s in nematics (discotics) and

smectics C. The spontaneously broken symmetry in cholesterics is the translational symmetry along the pitch axis p, which can equally well be described as a rotation about this axis. The variable Ri has, there- fore, the Poisson bracket relations

(Pi, Li are total linear momentum and total angular

momentum, respectively). The frequency matrix ele- ment

describes the instantaneous reversible dynamic cou- pling of R and the momentum density g (or the velo- city V) given by equation (6.1). Using a coarse grained

version of R(r) namely

in order to allow Fourier transformation (cf Ref [23]),

we obtain

Equation (6.2) reproduces the structure of equa- tion (6 .1 ) and relates (the instantaneous part of) the

coefficients g 1 and g2 to the microscopic order para-

meter Am > Pm. The difference gl - g2 is non zero,

therefore, only due to the collision dominated parts of g 1 and g2, which we have neglected above.

References

[1] Yu, L. J. and SAUPE, A., Phys. Rev. Lett. 45 (1980)

1000.

[2] BRAND, H. and PLEINER, H., Phys. Rev. A 24 (1981)

2777.

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858

[3] SASLOW, W. M. (preprint).

[4] JACOBSON, E. A. and SWIFT, J. (preprint).

[5] LIU, M., Phys. Rev. A 24 (1981) 2720.

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

[7] FORSTER, D., Phys. Rev. Lett. 32 (1974) 1161.

[8] PRIEST, R. G. and LUBENSKY, T. C., Phys. Rev. A 9 (1974) 893.

[9] STRALEY, J. P., Phys. Rev. A 10 (1974) 1881.

[10] CHANDRASEKHAR, S., SADASHIRA, B. K. and SURESH, K.

A., Pramana 9 (1977) 471.

[11] See e.g. the articles of BILLARD, J., GASPAROUX, H.

and LEVELUT, G. P., in Liquid Crystals of One-

and Twodimensional Order, edited by W. Hel-

frich and G. Heppke (Springer, Berlin) 1980.

[12] TINH, N. H., MALTHÈTE, J. and DESTRADE, C., J.

Physique-Lett. 42 (1981) L-417.

[13] DESTRADE, C., BERNAUD, M. C., GASPAROUX, H., LEVELUT, A. M., TINH, N. H., in Liquid Crys- tals, Proc. of the Intern. Conference on Liquid Crystals, ed. by S. Chandrasekhar (Heyden, Philadelphia) 1980.

[14] DESTRADE, C., TINH, N. H., MALTHÈTE, J. and JAQUES, J., Phys. Lett. A 79 (1980) 189.

[15] FUGNITTO, R., STRZELECKA, H., ZANN, A., DUBOIS, J. C. and BILLARD, J., J.C.S. Chem. Comm. 271

(1980).

[16] MARTIN, P. C., PARODI, O. and PERSHAN, P. S., Phys.

Rev. A 6 (1972) 2401.

[17] BRAND, H. and PLEINER, H., J. Physique 41 (1980) 553.

[18] FORSTER, D., Ann. Phys. (New York) 84 (1974) 505.

[19] For a hydrodynamic theory cf. PROST, J. and CLARK,

N. A., in the books cited in references [11] and [13]

and BRAND, H. and PLEINER, H. [2].

[20] VOLOVIK, G. E., JETP Lett. 31 (1980) 273.

[21] LUBENSKY, T. C., Phys. Rev. A 6 (1972) and Mol.

Cryst. Liq. Cryst. 23 (1973) 99.

[22] For a possible experimental evaluation of these coeffi-

cients, cf. JANOSSY, I., J. Physique-Lett. 42 (1981) L-43, and

BRAND, H. and PLEINER, H., J. Physique-Lett. 42 (1981) L-327.

[23] FORSTER, D., Hydrodynamic Fluctuations, Broken Sym-

metries, and Correlation Functions (Benjamin,

Reading) 1975.

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