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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�
573
Optical properties of anisotropic periodic helical
structuresC. 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 awide class of
optically anisotropic
media, characterizedby
aperiodicity along
one direction,generated by
a uniform rotation of the dielectric tensor around this axis.
Many
structures are known, which aresuitably
described
by
such anoptical
model. Thesimplest
ones are the twisted nematics and the cholesteric
liquid crystals
(N*), where one of theprincipal optical
axes of the dielectric tensor is
parallel
to the rotationaxis.
The general case
corresponds
however to morecomplicated
structures, i.e. to some smecticphases.
Among
them, the mostwidely
studied systems are the chiral C-smectics(S*)
which are constitutedby
Article published online by EDP Sciences and available at http://dx.doi.org/10.1051/jphys:01985004604057300
monolayers
ofprolate-shaped
molecules whoselong
axes are tilted
by
a constant angle with respect to the normal to thelayers.
Thetypical
helicoidal struc- ture of thisphase originates
from the presence of aprogressive,
uniform rotation of thelong
axes of themolecules of different
planes
around the normal to the set oflayers,
which is the helical axis of the struc- ture (and the z-axis of a suitable referenceframe).
The rotation of molecules is
completed
in one fullpitch length p,
which is here coincident with thespatial periodicity
of the structure. In cholestericliquid crystals,
thisperiodicity
is insteadp j2.
The optical
properties
of theseanisotropic
mediaare very
peculiar
andinteresting
from different view-points.
Most of the papers
published
so far are concernedwith theoretical and
experimental
studies of thepropagation
oflight along
the z-axis.Although
thisis
only
aspecial
case, it is in fact of great interest both intheory
andapplication.
A very extensive literatureexists,
particularly
in the case of cholestericliquid crystals.
Detailed references can be found in recentcomprehensive
reviews [1, 2].As far as the
light propagation
is along the z-axis,smectic
liquid
crystals neither show newoptical properties
nor pose substantialanalytical problems
with respect to cholesterics [3-5]. Difficulties arise instead in the case of
light obliquely propagating
withrespect to the helical axis of the structure.
Berreman
numerically
solved the Maxwell equa- tions forS*
in thegeneral
case ofoblique
incidence,and calculated in a direct way the reflection spectra of model
S*
and N*samples having
surfaces normal to the helical axis[3].
Inoblique
incidence, the reflec- tion and transmission spectra of these structures arerather different. In particular, a second set of Bragg
reflection
peaks
adds up, inS*,
to the set presentin cholesteric
liquid crystals.
Thisprediction
has beenexperimentally
verified [6, 7].While
simple inspection
of thesymmetries
of thestarting
set of Maxwell’sequations
used in numericalcomputation
is sufficient toexplain
the presence and location of the reflection bands in both cases, the number and thepolarization properties
of thepeaks
of each band cannot be
adequately interpreted
withoutexplicitly considering
the details of wavepropagation
in these
crystals.
This is done hereby considering
theelectromagnetic
wave as asuperposition
ofeigen-
modes, which are the Bloch wavescorresponding
tothe
periodic
structure under consideration. This method has the obvious advantage, over numericalapproaches,
ofgiving extremely
detailed information aboutlight propagation
within thecrystal.
Further-more, it
provides
adeeper understanding
of resultsreferring
tospecific optical properties,
such astypically
the behaviour of the reflectance as a function of the
wavelength
of incidentlight.
As a matter of fact, this
general
approach has beenapplied
so far to the case of cholestericliquid crystals,
allowing
various features oflight propagation
inthese systems
[8-12]
to be studied in detail. The closeanalogy existing
betweenS*
and N* structures sug-gests that a similar
approach
should be suitable also in the case of chiral smecticcrystals.
However, thestriking
differences observed inlight propagation
between
S*
and N* structuresimply
that thestudy
of the
S* crystals
cannot bemerely
considered as astraightforward
extension of the formalismdeveloped
to
investigate
cholestericliquid crystals,
but deservesa
fully independent
treatment.To our
knowledge,
theonly existing theory
forS*
structures,
explicitly following
this line ofapproach,
was
proposed by Taupin et
al. [13], who establisheda 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, thedispersion
relations of theindependent eigen-
modes of the
problem
are insteadgiven
in the form ofan
analytical
characteristicequation,
which is derivedby taking
into account all the essentialsymmetries
of the
problem.
Theoptical properties
of the structureare 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 smecticliquid crystal having
planar surfaces normal to the helical axis. Let (x, y, z) be a reference frame such that thesample
surfaces areparallel
to the (x,y)
plane, thehelical axis of the
liquid
crystalbeing along
the z-axis.The
optical properties
inS*’s
are determined, atany
point, by
the local dielectric tensor, i.e.by
itsprincipal
values E1, E2, 83 andby
thecorresponding 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 Eulerangles
(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 0and 03C8
have constant values,while
is
proportional
to z,going through
2 nc radians in onefull
pitch length,
p ; i.e.~>
= qzwith q
=2 nIp.
Thecomponents in the (x, y, z) frame of the dielectric tensor have been evaluated
by
Berreman [3]. In the present paper it isassumed ql
= 0. For these condi-tions, the dielectric tensor
E(~)
can be written, when4> = 0 as :
575
As a consequence, E can be
expressed,
forarbitrary 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 thatprecisely
these terms are characterizedby
adifferent
periodicity
with respect to the other z-dependent
elements of the tensor. This feature has relevant consequences on thedegree
ofcomplexity
of the formalism needed to
study light propagation
in
S*. According
to Berreman[3],
Maxwell’sequations
for
plane
waves inS*
can be written aswhere c and m are the
velocity
andfrequency
of theincident
light,
T is the column 4 vector and d isthe 4 x 4 matrix :
By
making
use ofequations
(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 oflight
on thesample’s
surface.In addition :
Equation (4)
can be solvednumerically [3].
However,a
deeper knowledge
of the details of wavepropagation
in
S*,
inspite
of thecomplexity
of their structure andof the
corresponding
mathematical formalism, may be obtainedby explicitly taking
into account the existingsymmetries
of theproblem.
Inparticular,
the transla- tional symmetry of the structurealong
any directionperpendicular
to the helical axis suggests that the solutions ofequation
(4), forplane
wavepropagation
inthe (x, z) plane, will take the form :
where both E(z) and
H(z)
areonly
functions of z.The
wavevector kx
is related to m = ni sin0; by
therelation m =
kx c/m.
By
using
thefollowing
relations forHx
andHy (easily
obtained fromequations
(4) and(5)) :
the set of linear
equations
(4) can be reduced to apair
ofcoupled,
second-order differentialequations
for thefield components
Ex, Ey :
The
periodicity
of the structurealong
the z-axis allows the solutions ofequation
(11) to be written in the form :i.e. as
superpositions
of Fourier components,according
to theBloch-Floquet
theorem. Inequation
(12)kz
is thecomponent,
parallel
to the helical axis, ofthe
wavevector of incidentlight.
Substitution ofequation (12)
in thecoupled
difterentialequations (11) gives
rise to an infinite set ofalgebraic equations
for the unknowns(x,,, y,,) :
where
The form of
equation (12)
is such that inequations
(13)all the coefficients of the unknown
(xn, y")
are realfunctions
of kz
if the medium is nondissipative,
i.e. if thedielectric tensor is real. The infinite set (13) of homo-
geneous
equations
for the unknownquantities (x", y,,)
admits nontrivial solutions if and
only
if the deter-minant of coefficients, D,
regarded
as a function of thecomplex
variablekZ,
isequal
to zero. This conditiongives
the secularequation,
from which both inde-pendent eigenvalues
can besimultaneously
obtainedfor any value of the
frequency
of the incidentlight.
The set
(13)
isremarkably
more involved than thethree-diagonal
setcorresponding
to the case ofcholesteric
liquid crystals.
For this reason the ad hocmethods used in references
[9,
10] to find theeigen-
values of the
three-diagonal
setcorresponding
to thecase of a N* cannot be
directly applied
to the moregeneral
case of aSg.
In reference[13)
apurely
numericiterative
procedure
issuggested.
This method isclearly
not suitable in the cases where theeigenvalues
of the
equation
system aredegenerate
ornearly degenerate,
as for instance near the boundaries of the reflection bands.In the next section a
simple analytical
form for the secularequation
isgiven.
In thisequation,
which is the characteristicequation
of theproblem,
all essential symmetryproperties
of theproblem
areclearly
shown.This is the main
advantage
of the present method over allprevious
attempts. The coefficients which appear in the characteristicequation
arestraightforwardly
deduced from the coefficients of the recurrent relations
(13),
thusavoiding
any iterationprocedure.
3. Characteristic
equation
for the eigenmodes.The
problem
ofobtaining
thedispersion
relationskz(w)
for theeigenmodes (xn, yn)
ofelectromagnetic
waves
propagating
within theS*
may besuitably
reduced to the
analysis
of the solutions of asimple biquadratic equation
for the variable sin nk, wherek =
k2/q.
This is the centralpoint
of the presentapproach,
and represents a remarkableimprovement
with respect to conventional methods of numerical
computation.
The characteristic
equations
readswhere the functions U and V can be obtained, in terms
of
D(k), through
standardapplication
of an ad hoc formalism,expressly developed
to solve theproblem
of
light propagation
inperiodic
structures, whose main features are summarized in thefollowing.
For furthermathematical details, the reader is referred to paper
[11]
]and to references therein. First, the convergency of the
577
coefficients’ determinant
D (k)
is ensuredby
alterna-tively dividing
the recurrent relations,(13a)
and(13b) by
thequantities An
andB., respectively.
One obtains anew coefficients’ determinant
D * (k)
in which all the main diagonal elementsDn
are unity.Two
auxiliary
functionsda and db
may now be defined aswhere both limits (k -->
ka, k -+ k6)
can be shown toexist and to be
generally
nonzero, sinceD *(k)
turnsout to be an
analytical
function of thecomplex
variable k, with four infinite sets of
simple poles
on thereal k-axis, for k =
± kp
+ n and k =1: kb
+ n (n =integer).
In particular, D * (k)diverges
as1 l(k - k.,b) when k -> ku,b.
Finally,
the U and V functions aregiven by
In
principle,
the fourindependent
roots of equa- tion(15) give
rise to four infinite sets of k values,which are the
eigenvalues
of theproblem :
However a change of n
merely corresponds
to a re-indexing
of the unknowns x,,,y,, and kt, Ki
corres-pond
to wavespropagating
forwards and backwardsrespectively.
As a consequence, for eachpoint
of the (w,0;) plane,
i.e. for eachfrequency
of incidentlight
and each
angle
of incidenceOi, only
tworeally
inde-pendent
modes are excited,corresponding
to theeigenvalues k1 and k2 respectively.
It can be
easily
shown that three different types of solutions of the characteristicequation (15)
may occur,depending
on the values of the coefficients U(co,Oi)
and F(co,
Oi). Actually,
theresulting eigenvalues k,,2
may
independently
be either real orcomplex.
Areal k
corresponds
to apropagating
wave i.e. to a stablesolution. A
complex ki corresponds
to an attenuatedwave, i.e. to an unstable solution. Two different types of instabilities can occur
depending
on the value takenby
the real part of k which,according
to reference [11]are referred as B- and
C-type
instabilitiesrespectively.
In both cases, the
instability
occurs where the wavesreflected from
layers
which are onepitch
apart addcoherently, giving
rise to a strong reflection. In case B, only one mode is involved, the incident and reflectedwaves
having opposite k
values. The realpart k’
of ktherefore 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 botheigenmodes
arenecessarily
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, thepolariza-
tion states of the incident and reflected
light
arealmost
opposite (either
from mode 7r to mode Q, or vice versa, astypically
inS*
and in N* atsufficiently high
incidenceangles,
or from left toright
circularpolarization,
or vice versa, as in N* at lower incidenceangles).
This case ismathematically
characterizedby
anegative
value of the discriminant of the characteristicequation (15),
so that theBragg
condition is nolonger
satisfied. A
physically quite
similar situation occursif both
eigenmodes simultaneously undergo
aB-type instability
with total reflection of the incidentlight.
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 acomplete
classification of its solution can be found in reference[12].
4. Structure of the Bragg reflection bands.
The formalism
developed
in theprevious
sectionsallows one to
perform
a detailedanalysis
oflight propagation
in a wide class ofliquid crystals. Actually, setting
0 =n/2
in thedefining equations
for thedielectric tensor is
equivalent
toconsidering
aperfect
cholesteric
liquid crystal.
On the other hand,by setting
0=0and 81
= 82 one obtains a homogeneousmedium. Intermediate values of the tilt
angle
0obviously
describe different chiral smecticliquid crystals.
Within the present framework, it is thenpossible
to follow in great detail the behaviour of thedispersion
relations of a set ofS*, by continuously varying
asingle
parameter, 0, between the limits above described.Typical examples
of the results which can be extracted from the presentapproach
are reportedin the
following.
First the solution of the characteristicequation
areanalysed
and both the real andimaginary
part of the
independent eigenvalues k,,2
areplotted
asfunctions of
plA
= wlqc. A reduced Brillouin zonescheme is used throughout. The
principal
values of the dielectric tensoralways
are 81 = B2 = 2, E3 = 3.These values are coincident with those used in Berre- man’s paper
[3]. Figures
2 to 5 describe thedispersion
relations of a set of different structures with
decreasing
tilt angles (0 = 90°, 75°, 45°, 150), for
obliquely
inci-dent
light.
For the sake ofsimplicity,
and in order to evidence thedependence
on 0 of thedispersion
relations, theangle
of incidenceOi
waskept
constantand
equal
to 60° for all curves.Figure
2 shows thetypical
behaviour of thedisper-
sion curves of a
perfect
cholestericliquid crystal
(0 = 90°) athigh
incidenceangle
and for afrequency
range
corresponding
to the first two reflection bands.Each band is a
triplet,
whose externalpeaks
are dueto the
Bragg
reflection of each one of the two inde-pendent
eigenmodes
(andcorrespond
to the B-typeinstabilities of the two
dispersion
curves), while thecentral
peak
is a total reflectionpeak (corresponding
to the
C-type instability,
which is common to bothdispersion
curves; notice that the real part of k does notsatisfy
the Bragg condition, i.e. 2 k’ :Ainteger).
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 patternanalysed
in
figure
2. This new set ofinstability regions
derives,as is indeed
expected,
from the terms of thestarting equations,
which contain theperiodicity 0
= qz inaddition to the
periodicity 0
= 2 qz. As a consequence, thedispersion
relations of anS* crystal
atoblique
incidence look rather more
complicated
than thoseof a N* in the same conditions. As a matter of fact,
the set of
peaks
of k",intrinsically
associated with theperiodicity
qz, becomes ofincreasing
relevance with respect the other set when 0 decreases. For 0 = 15°,corresponding
to anearly homogeneous
medium,only
the firstpeak
of k" issignificantly
present, thedispersion
curves for k’being
rathersimple,
asexpected.
The
instability regions
intrisic toS*
possess remar- kable features. These are in fact isolated pureC-type
instabilities, while those associated with the 2 qzperiodicity
arecomposed
of B-C-B, or B-(B + B)-Btriplets
[11]. In other words, no additional B-typereflection
peaks
turn out to be related to the qzperiodicity
of the system. It seemsinteresting
toanalyse
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 firstinstability region,
the twoindependent
branches of thedispersion
relationscorrespond
to almostlinearly polarized eigenmodes.
Inparticular,
the upper branch is associated with mode Q, the lower one to mode n.This
polarization
state is well defined andpreserved
until the first
instability region
isapproached.
At agiven
valueof plA,
theupper k
branchactually
crossesthe line k’ =
1/2.
However no B-type band appears, thecorresponding
k"remaining identically
zero there.Finally,
in the reduced Brillouin zone scheme bothindependent
modescollapse
and sticktogether,
defin-ing
atypical C-type
reflectionpeak.
Within thepeak,
a mode
mixing
occurs, aspreviously
discussed. On theopposite
side of thepeak,
the modesagain
becomedistinguishable
and stable, theirpolarizations being
now reversed. The
upper k’
branch,corresponding
now to mode n, will cross the line k’ =
1/2, again
without
generating
a B-typeinstability.
Fig. 4. - Same as figure 2, with 8 = 45°.