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HAL Id: jpa-00209997

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Submitted on 1 Jan 1985

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Optical properties of anisotropic periodic helical structures

C. Oldano, P. Allia, L. Trossi

To cite this version:

C. Oldano, P. Allia, L. Trossi. Optical properties of anisotropic periodic helical structures. Journal de Physique, 1985, 46 (4), pp.573-582. �10.1051/jphys:01985004604057300�. �jpa-00209997�

(2)

573

Optical properties of anisotropic periodic helical

structures

C. Oldano (*,°), P. Allia

(+,°)

and L. Trossi

(*)

(*) Dipartimento di Fisica, Politecnico di Torino, Italy (+) Istituto Elettrotecnico Nazionale G. Ferraris, Torino, Italy

(°) Gruppo Nazionale Struttura della Materia del C.N.R., U.R. 24 Torino, Italy

(Reçu le 6 août 1984, accepté le 22 novembre 1984)

Résumé. 2014 On considère un modèle optique décrivant une large classe de milieux optiquement anisotropes tels

que les cristaux liquides smectiques chiraux et, à la limite, les cristaux liquides cholestériques et les milieux homo-

gènes anisotropes. Ce modèle décrit une structure présentant une périodicité le long d’un axe donné, engendrée

par une rotation uniforme du tenseur diélectrique. Les équations de Maxwell étudiées jusqu’à présent seulement

pour des cas particuliers sont résolues ici dans le cas général où la direction de propagation des ondes et l’orientation de l’axe de rotation du tenseur diélectrique forment un angle arbitraire. Le processus de résolution met en jeu le

calcul des modes propres de l’onde électromagnétique, c’est-a-dire les ondes de Bloch propres à la structure pério- dique, qui se réduit aux ondes ordinaires et extraordinaires dans le cas limite d’une structure homogène anisotrope.

De la relation de dispersion des modes propres ainsi déduits on tire les propriétés optiques de cette structure sur une base générale. Les bandes de réflexion de Bragg sont formées d’une alternance de singulets et de triplets. En général, les bandes d’ordre pair sont des triplets dont les pics latéraux correspondent aux instabilités de Bragg

des modes propres considérés tandis que le pic central est commun aux deux modes propres et conduit à la réflexion totale avec échange de mode. Les bandes d’ordre impair sont formées de singulets dont les caractéristiques sont

très voisines de celles du pic central des triplets. Les propriétés de polarisation des modes propres sont étudiées dans le cas particulier d’un milieu localement uniaxe pour lequel les ondes de Bloch présentent un brusque chan-

gement de polarisation à une valeur particulière de l’angle entre l’axe optique et l’axe de rotation.

Abstract 2014 An optical model is considered describing a wide class of optically anisotropic media such as chiral smectic liquid crystals and, in the limiting cases, cholesteric liquid crystals and anisotropic homogeneous media.

It describes a structure having a periodicity along a given axis generated by a uniform rotation of the dielectric tensor. Maxwell’s equations for this model, studied so far only in particular cases, are here solved for the general

case where the direction of the propagating waves and the orientation of the dielectric tensor make an arbitrary angle with respect to the rotation axis. The resolving procedure involves the evaluation of the eigenmodes of the electromagnetic wave, i.e. the Bloch waves intrinsic to the specific periodic structure, which reduce to the ordinary

and extraordinary waves in the limiting case of anisotropic homogeneous structures. The dispersion relation for

the eigenmodes is deduced, allowing the study of the optical properties of this structure on a general basis. The Bragg reflection bands are found to be constituted alternatively by singlets and triplets. In general the even order bands are triplets whose lateral peaks correspond to the Bragg instabilities of each eigenmode, while the central

peak is common to both eigenmodes and gives total reflection with a mode exchange. The odd order bands are singlets whose characteristics are very similar to the central peak of the triplets. The polarization properties of the eigenmodes are studied in the particular case of locally uniaxial media, where the Bloch waves show an abrupt polarization change for a particular value of the angle between the optical axis and the rotation axis.

J. Physique 46 (1985) 573-582 AVRIL 1985,

Classification

Physics Abstracts

41.10H 2013 61.30 - 42.10Q

1. Introduction.

Considerable attention has

recently developed

for a

wide class of

optically anisotropic

media, characterized

by

a

periodicity along

one direction,

generated by

a uniform rotation of the dielectric tensor around this axis.

Many

structures are known, which are

suitably

described

by

such an

optical

model. The

simplest

ones are the twisted nematics and the cholesteric

liquid crystals

(N*), where one of the

principal optical

axes of the dielectric tensor is

parallel

to the rotation

axis.

The general case

corresponds

however to more

complicated

structures, i.e. to some smectic

phases.

Among

them, the most

widely

studied systems are the chiral C-smectics

(S*)

which are constituted

by

Article published online by EDP Sciences and available at http://dx.doi.org/10.1051/jphys:01985004604057300

(3)

monolayers

of

prolate-shaped

molecules whose

long

axes are tilted

by

a constant angle with respect to the normal to the

layers.

The

typical

helicoidal struc- ture of this

phase originates

from the presence of a

progressive,

uniform rotation of the

long

axes of the

molecules of different

planes

around the normal to the set of

layers,

which is the helical axis of the struc- ture (and the z-axis of a suitable reference

frame).

The rotation of molecules is

completed

in one full

pitch length p,

which is here coincident with the

spatial periodicity

of the structure. In cholesteric

liquid crystals,

this

periodicity

is instead

p j2.

The optical

properties

of these

anisotropic

media

are very

peculiar

and

interesting

from different view-

points.

Most of the papers

published

so far are concerned

with theoretical and

experimental

studies of the

propagation

of

light along

the z-axis.

Although

this

is

only

a

special

case, it is in fact of great interest both in

theory

and

application.

A very extensive literature

exists,

particularly

in the case of cholesteric

liquid crystals.

Detailed references can be found in recent

comprehensive

reviews [1, 2].

As far as the

light propagation

is along the z-axis,

smectic

liquid

crystals neither show new

optical properties

nor pose substantial

analytical problems

with respect to cholesterics [3-5]. Difficulties arise instead in the case of

light obliquely propagating

with

respect to the helical axis of the structure.

Berreman

numerically

solved the Maxwell equa- tions for

S*

in the

general

case of

oblique

incidence,

and calculated in a direct way the reflection spectra of model

S*

and N*

samples having

surfaces normal to the helical axis

[3].

In

oblique

incidence, the reflec- tion and transmission spectra of these structures are

rather different. In particular, a second set of Bragg

reflection

peaks

adds up, in

S*,

to the set present

in cholesteric

liquid crystals.

This

prediction

has been

experimentally

verified [6, 7].

While

simple inspection

of the

symmetries

of the

starting

set of Maxwell’s

equations

used in numerical

computation

is sufficient to

explain

the presence and location of the reflection bands in both cases, the number and the

polarization properties

of the

peaks

of each band cannot be

adequately interpreted

without

explicitly considering

the details of wave

propagation

in these

crystals.

This is done here

by considering

the

electromagnetic

wave as a

superposition

of

eigen-

modes, which are the Bloch waves

corresponding

to

the

periodic

structure under consideration. This method has the obvious advantage, over numerical

approaches,

of

giving extremely

detailed information about

light propagation

within the

crystal.

Further-

more, it

provides

a

deeper understanding

of results

referring

to

specific optical properties,

such as

typically

the behaviour of the reflectance as a function of the

wavelength

of incident

light.

As a matter of fact, this

general

approach has been

applied

so far to the case of cholesteric

liquid crystals,

allowing

various features of

light propagation

in

these systems

[8-12]

to be studied in detail. The close

analogy existing

between

S*

and N* structures sug-

gests that a similar

approach

should be suitable also in the case of chiral smectic

crystals.

However, the

striking

differences observed in

light propagation

between

S*

and N* structures

imply

that the

study

of the

S* crystals

cannot be

merely

considered as a

straightforward

extension of the formalism

developed

to

investigate

cholesteric

liquid crystals,

but deserves

a

fully independent

treatment.

To our

knowledge,

the

only existing theory

for

S*

structures,

explicitly following

this line of

approach,

was

proposed by Taupin et

al. [13], who established

a set of

equations

for the coefficients of Bloch waves.

However, this set was solved

only numerically by

means of an iterative

procedure.

In the present paper, the

dispersion

relations of the

independent eigen-

modes of the

problem

are instead

given

in the form of

an

analytical

characteristic

equation,

which is derived

by taking

into account all the essential

symmetries

of the

problem.

The

optical properties

of the structure

are then discussed on a much firmer basis. In

particular

the features of the reflection bands are

fully analysed

and their most

important polarization properties

evidenced.

2. Propagation equations.

Let us consider a

sample

of a chiral smectic

liquid crystal having

planar surfaces normal to the helical axis. Let (x, y, z) be a reference frame such that the

sample

surfaces are

parallel

to the (x,

y)

plane, the

helical axis of the

liquid

crystal

being along

the z-axis.

The

optical properties

in

S*’s

are determined, at

any

point, by

the local dielectric tensor, i.e.

by

its

principal

values E1, E2, 83 and

by

the

corresponding principal

directions, which define a local frame (1, 2, 3).

Transformation from (x, z, z) to (1, 2, 3) is

performed by properly rotating

(x, y, z)

by

the set of Euler

angles

(0,

4>, 03C8)

defined in reference [3].

Specifically,

three successive rotations are involved,

as shown in

figure

1 : a) By 0 around the x-axis.

b)

By ql

around the 3-axis. c)

By 0

around the z-axis.

In

S*

both 0

and 03C8

have constant values,

while

is

proportional

to z,

going through

2 nc radians in one

full

pitch length,

p ; i.e.

~>

= qz

with q

=

2 nIp.

The

components in the (x, y, z) frame of the dielectric tensor have been evaluated

by

Berreman [3]. In the present paper it is

assumed ql

= 0. For these condi-

tions, the dielectric tensor

E(~)

can be written, when

4> = 0 as :

(4)

575

As a consequence, E can be

expressed,

for

arbitrary 0

values as :

where

The structure of this tensor differs from that for cholesteric

liquid crystals

because of the terms Exz, Byz, which are nonzero in the present case. Let us notice that

precisely

these terms are characterized

by

a

different

periodicity

with respect to the other z-

dependent

elements of the tensor. This feature has relevant consequences on the

degree

of

complexity

of the formalism needed to

study light propagation

in

S*. According

to Berreman

[3],

Maxwell’s

equations

for

plane

waves in

S*

can be written as

where c and m are the

velocity

and

frequency

of the

incident

light,

T is the column 4 vector and d is

the 4 x 4 matrix :

By

making

use of

equations

(1) and (2), the elements of A can be written :

where

ni is the refraction index of the external medium

and 0;

the

angle

of incidence of

light

on the

sample’s

surface.

In addition :

Equation (4)

can be solved

numerically [3].

However,

a

deeper knowledge

of the details of wave

propagation

in

S*,

in

spite

of the

complexity

of their structure and

of the

corresponding

mathematical formalism, may be obtained

by explicitly taking

into account the existing

symmetries

of the

problem.

In

particular,

the transla- tional symmetry of the structure

along

any direction

perpendicular

to the helical axis suggests that the solutions of

equation

(4), for

plane

wave

propagation

in

the (x, z) plane, will take the form :

where both E(z) and

H(z)

are

only

functions of z.

The

wavevector kx

is related to m = ni sin

0; by

the

relation m =

kx c/m.

By

using

the

following

relations for

Hx

and

Hy (easily

obtained from

equations

(4) and

(5)) :

the set of linear

equations

(4) can be reduced to a

pair

of

coupled,

second-order differential

equations

for the

field components

Ex, Ey :

(5)

The

periodicity

of the structure

along

the z-axis allows the solutions of

equation

(11) to be written in the form :

i.e. as

superpositions

of Fourier components,

according

to the

Bloch-Floquet

theorem. In

equation

(12)

kz

is the

component,

parallel

to the helical axis, of

the

wavevector of incident

light.

Substitution of

equation (12)

in the

coupled

difterential

equations (11) gives

rise to an infinite set of

algebraic equations

for the unknowns

(x,,, y,,) :

where

The form of

equation (12)

is such that in

equations

(13)

all the coefficients of the unknown

(xn, y")

are real

functions

of kz

if the medium is non

dissipative,

i.e. if the

dielectric tensor is real. The infinite set (13) of homo-

geneous

equations

for the unknown

quantities (x", y,,)

admits nontrivial solutions if and

only

if the deter-

minant of coefficients, D,

regarded

as a function of the

complex

variable

kZ,

is

equal

to zero. This condition

gives

the secular

equation,

from which both inde-

pendent eigenvalues

can be

simultaneously

obtained

for any value of the

frequency

of the incident

light.

The set

(13)

is

remarkably

more involved than the

three-diagonal

set

corresponding

to the case of

cholesteric

liquid crystals.

For this reason the ad hoc

methods used in references

[9,

10] to find the

eigen-

values of the

three-diagonal

set

corresponding

to the

case of a N* cannot be

directly applied

to the more

general

case of a

Sg.

In reference

[13)

a

purely

numeric

iterative

procedure

is

suggested.

This method is

clearly

not suitable in the cases where the

eigenvalues

of the

equation

system are

degenerate

or

nearly degenerate,

as for instance near the boundaries of the reflection bands.

In the next section a

simple analytical

form for the secular

equation

is

given.

In this

equation,

which is the characteristic

equation

of the

problem,

all essential symmetry

properties

of the

problem

are

clearly

shown.

This is the main

advantage

of the present method over all

previous

attempts. The coefficients which appear in the characteristic

equation

are

straightforwardly

deduced from the coefficients of the recurrent relations

(13),

thus

avoiding

any iteration

procedure.

3. Characteristic

equation

for the eigenmodes.

The

problem

of

obtaining

the

dispersion

relations

kz(w)

for the

eigenmodes (xn, yn)

of

electromagnetic

waves

propagating

within the

S*

may be

suitably

reduced to the

analysis

of the solutions of a

simple biquadratic equation

for the variable sin nk, where

k =

k2/q.

This is the central

point

of the present

approach,

and represents a remarkable

improvement

with respect to conventional methods of numerical

computation.

The characteristic

equations

reads

where the functions U and V can be obtained, in terms

of

D(k), through

standard

application

of an ad hoc formalism,

expressly developed

to solve the

problem

of

light propagation

in

periodic

structures, whose main features are summarized in the

following.

For further

mathematical details, the reader is referred to paper

[11]

]

and to references therein. First, the convergency of the

(6)

577

coefficients’ determinant

D (k)

is ensured

by

alterna-

tively dividing

the recurrent relations,

(13a)

and

(13b) by

the

quantities An

and

B., respectively.

One obtains a

new coefficients’ determinant

D * (k)

in which all the main diagonal elements

Dn

are unity.

Two

auxiliary

functions

da and db

may now be defined as

where both limits (k -->

ka, k -+ k6)

can be shown to

exist and to be

generally

nonzero, since

D *(k)

turns

out to be an

analytical

function of the

complex

variable k, with four infinite sets of

simple poles

on the

real k-axis, for k =

± kp

+ n and k =

1: kb

+ n (n =

integer).

In particular, D * (k)

diverges

as

1 l(k - k.,b) when k -> ku,b.

Finally,

the U and V functions are

given by

In

principle,

the four

independent

roots of equa- tion

(15) give

rise to four infinite sets of k values,

which are the

eigenvalues

of the

problem :

However a change of n

merely corresponds

to a re-

indexing

of the unknowns x,,,

y,, and kt, Ki

corres-

pond

to waves

propagating

forwards and backwards

respectively.

As a consequence, for each

point

of the (w,

0;) plane,

i.e. for each

frequency

of incident

light

and each

angle

of incidence

Oi, only

two

really

inde-

pendent

modes are excited,

corresponding

to the

eigenvalues k1 and k2 respectively.

It can be

easily

shown that three different types of solutions of the characteristic

equation (15)

may occur,

depending

on the values of the coefficients U(co,

Oi)

and F(co,

Oi). Actually,

the

resulting eigenvalues k,,2

may

independently

be either real or

complex.

A

real k

corresponds

to a

propagating

wave i.e. to a stable

solution. A

complex ki corresponds

to an attenuated

wave, i.e. to an unstable solution. Two different types of instabilities can occur

depending

on the value taken

by

the real part of k which,

according

to reference [11]

are referred as B- and

C-type

instabilities

respectively.

In both cases, the

instability

occurs where the waves

reflected from

layers

which are one

pitch

apart add

coherently, giving

rise to a strong reflection. In case B, only one mode is involved, the incident and reflected

waves

having opposite k

values. The real

part k’

of k

therefore satisfies the Bragg condition : 2 k’ = 0,

± 1, ± 2, ... In case C instead, the coherent reflection is the one that gives rise to a mode

exchange,

so that both

eigenmodes

are

necessarily

involved, and total reflec-

Fig. 1. - Euler angles of the dielectric tensor principal axes (1, 2, 3) with respect to the sample (x, y, z) frame (after Berreman, Ref. 3).

tion of incident

light

occurs. In this case, the

polariza-

tion states of the incident and reflected

light

are

almost

opposite (either

from mode 7r to mode Q, or vice versa, as

typically

in

S*

and in N* at

sufficiently high

incidence

angles,

or from left to

right

circular

polarization,

or vice versa, as in N* at lower incidence

angles).

This case is

mathematically

characterized

by

a

negative

value of the discriminant of the characteristic

equation (15),

so that the

Bragg

condition is no

longer

satisfied. A

physically quite

similar situation occurs

if both

eigenmodes simultaneously undergo

a

B-type instability

with total reflection of the incident

light.

In this case, too, the

polarization

state of the incident and reflected beams can be very different.

A more detailed discussion of

equation (15)

and a

complete

classification of its solution can be found in reference

[12].

4. Structure of the Bragg reflection bands.

The formalism

developed

in the

previous

sections

allows one to

perform

a detailed

analysis

of

light propagation

in a wide class of

liquid crystals. Actually, setting

0 =

n/2

in the

defining equations

for the

dielectric tensor is

equivalent

to

considering

a

perfect

cholesteric

liquid crystal.

On the other hand,

by setting

0=0

and 81

= 82 one obtains a homogeneous

medium. Intermediate values of the tilt

angle

0

obviously

describe different chiral smectic

liquid crystals.

Within the present framework, it is then

possible

to follow in great detail the behaviour of the

dispersion

relations of a set of

S*, by continuously varying

a

single

parameter, 0, between the limits above described.

Typical examples

of the results which can be extracted from the present

approach

are reported

in the

following.

First the solution of the characteristic

(7)

equation

are

analysed

and both the real and

imaginary

part of the

independent eigenvalues k,,2

are

plotted

as

functions of

plA

= wlqc. A reduced Brillouin zone

scheme is used throughout. The

principal

values of the dielectric tensor

always

are 81 = B2 = 2, E3 = 3.

These values are coincident with those used in Berre- man’s paper

[3]. Figures

2 to 5 describe the

dispersion

relations of a set of different structures with

decreasing

tilt angles (0 = 90°, 75°, 45°, 150), for

obliquely

inci-

dent

light.

For the sake of

simplicity,

and in order to evidence the

dependence

on 0 of the

dispersion

relations, the

angle

of incidence

Oi

was

kept

constant

and

equal

to 60° for all curves.

Figure

2 shows the

typical

behaviour of the

disper-

sion curves of a

perfect

cholesteric

liquid crystal

(0 = 90°) at

high

incidence

angle

and for a

frequency

range

corresponding

to the first two reflection bands.

Each band is a

triplet,

whose external

peaks

are due

to the

Bragg

reflection of each one of the two inde-

pendent

eigenmodes

(and

correspond

to the B-type

instabilities of the two

dispersion

curves), while the

central

peak

is a total reflection

peak (corresponding

to the

C-type instability,

which is common to both

dispersion

curves; notice that the real part of k does not

satisfy

the Bragg condition, i.e. 2 k’ :A

integer).

Fig. 2. - Real and imaginary part, k’ and k", of the z-compo- nent of the reduced wavevector versus p/ À. for the following

set of parameters: 81 = E2 = 2, 83 = 3, tilt angle 8 = n/2,

incidence angle Oi = 60°. B and C indicate the type of the instability regions, n and a the dominant polarization

states of the eigenmodes.

Fig. 3. - Same as figure 2, with 0 = 75°. The indices of B and C refer to the order of the Bragg reflection bands.

In

figures

3-5, where 0 :0 900 a new set of reflection bands is observed to add up to the pattern

analysed

in

figure

2. This new set of

instability regions

derives,

as is indeed

expected,

from the terms of the

starting equations,

which contain the

periodicity 0

= qz in

addition to the

periodicity 0

= 2 qz. As a consequence, the

dispersion

relations of an

S* crystal

at

oblique

incidence look rather more

complicated

than those

of a N* in the same conditions. As a matter of fact,

the set of

peaks

of k",

intrinsically

associated with the

periodicity

qz, becomes of

increasing

relevance with respect the other set when 0 decreases. For 0 = 15°,

corresponding

to a

nearly homogeneous

medium,

only

the first

peak

of k" is

significantly

present, the

dispersion

curves for k’

being

rather

simple,

as

expected.

The

instability regions

intrisic to

S*

possess remar- kable features. These are in fact isolated pure

C-type

instabilities, while those associated with the 2 qz

periodicity

are

composed

of B-C-B, or B-(B + B)-B

triplets

[11]. In other words, no additional B-type

reflection

peaks

turn out to be related to the qz

periodicity

of the system. It seems

interesting

to

analyse

the reason for such behaviour.

Let us consider for instance the first

peak of figure

3.

At sufficiently low

frequencies,

i.e. well before the first

instability region,

the two

independent

branches of the

dispersion

relations

correspond

to almost

linearly polarized eigenmodes.

In

particular,

the upper branch is associated with mode Q, the lower one to mode n.

This

polarization

state is well defined and

preserved

until the first

instability region

is

approached.

At a

given

value

of plA,

the

upper k

branch

actually

crosses

the line k’ =

1/2.

However no B-type band appears, the

corresponding

k"

remaining identically

zero there.

Finally,

in the reduced Brillouin zone scheme both

independent

modes

collapse

and stick

together,

defin-

ing

a

typical C-type

reflection

peak.

Within the

peak,

a mode

mixing

occurs, as

previously

discussed. On the

opposite

side of the

peak,

the modes

again

become

distinguishable

and stable, their

polarizations being

now reversed. The

upper k’

branch,

corresponding

now to mode n, will cross the line k’ =

1/2, again

without

generating

a B-type

instability.

Fig. 4. - Same as figure 2, with 8 = 45°.

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