LIQUID CRYSTALS: Materials Displays: J. S. Patel

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Annu. Rev. Mater. Sci. 1993. 23:269-94

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LIQUID CRYSTALS: Materials for

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J. S. Patel
Bllcore, 331 NewmanSprings Road, Red Bank, NewJersey 07710
KEYWORDS: nematics,snaectic, electro-optic,ferroelectric effect, flexoelectric

effect
INTRODUCTION
It was about 100 years ago that an anomalyin the melting point of certain
materials led to the discovery of liquid crystals. An Austrian botanist
namedReinitzer had noticed that cholesteryl benzoate, a substance very
similar to cholesterol, did not melt at a precise temperatureas most organic
materials do. This curious behavior was thought to be due to impurity in
the material, but as the material was purified further, the anomalyin the
melting behavior grew, and led to the discovery of the first liquid crystal.
Withthis discovery of the cholesteric liquid crystal beganthe fascinating
search for other liquid crystals. Thewordcholesteric probably has its origin
in the fact that the material Reinitzer had investigated was a derivative of
cholesterol, and in liquid crystal becausethe material has a state in between
a liquid and a crystal. With discoveries that followed, it was learned that
cholesteric liquid crystals are actually a sub-class of a moregeneral class
of materials called nematics in which the molecules possess no positional
order, but have long range orientational order. By this we mean that
the long axis of the molecules remains approximately parallel over long
distances, but the position of the moleculesdoes not form a periodic lattice.
The local average direction of the long axis of the molecules is generally
represented by a unit vector, n, called the director. The nematic liquids
composedof chiral molecules or containing chiral additives possess a
helical structure and are called cholesteric liquid crystals. Liquid crystals
in general are sometimes called mesophases from the Greek word meso,
which means intermediate. It is remarkable that such a humblebeginning
269
0084-6600/93/0801-0269502.00
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270 PAT~L
would produce a several billion dollar market in the form of displays for
computers, televisions, calculators, and watches. In this review we examine
someof the liquid crystalline material properties, various electro-optic
effects, and the progress that has been madeto improveand optimize these
materials.
Liquid crystals are materials that have someproperties both of liquids
and of solids. They are anisotropic like some solids, and their physical
properties along different directions are generally different. For example,
these materials are birefringent and this optical anisotropy is easily
revealed by using a polarizing microscope. These materials also share

properties of liquids in that they are fluids. The commonnematic liquid

crystals have viscosity of the order of a poise, similar to that of oil. Like
the optical properties, the viscosity is also anisotropic. The smectics liquid
crystals have higher viscosities because of the higher degree of order.
Wefirst examinethe various types of liquid crystals that are possible.
As shown in Figure 1, they can be divided into two major classes; the
thermotropic and lyotropic liquid crystals. The thermotropic liquid crys-
tals changetheir properties with temperaturewhile lyotropic liquid crystals
are generally based on mixtures of two or more substances, one oi~ them
most often being water. These materials change their properties with
composition, but the properties also change with temperature. At present
there are no optical displays based on lyotropic liquid crystals and there-
fore these materials are not discussed here, although the interested reader
is referred to several interesting reviewarticles that describe their structure
and properties in great detail (1).
The thermotropic liquid crystals are generally divided into two classes,
LIQUID CRYSTALS
I I
thermotropic lyotropic
I
I I
rods discs
I
I
nematics smectics
,
smecticA
I
smectic B
I
smectic C
Figure1 Classificationof liquidcrystals.
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LIQUID CRYSTALS 271

the commonone being formed by liquid crystals composed of the rod-
shaped molecules. The other class is formed by the liquid crystals com-
posed of disc-shaped molecules (2), but these have not been used in display
devices(for a review, see Reference2). It is interesting to note that dividing
the materials into those with rod- and disc-shaped molecules that form
liquid crystalline phases is merely a matter of convenience. One might
imagine, for example, a dumb-bell-shaped molecule that resembles both a
rod as well as a disc, and may have properties somewherein between. In
fact, such molecules have bccn synthesized and do have liquid crystalline
properties (3).
Wcfocus on matcrials with rod-shaped molcculcs, which can bc sub-

divided into ncmatics or smcctics. Recent work on some materials has
madethis distinction blurry since certain newmaterials have characteristics
of both the nematic and smectics. The chief distinguishing feature between
the ncmatic and the smcctic is that the smcctic liquid crystals have micro-
scopic layered structures while the nematic have none.
Figure 2 depicts the nematic and the smectic phases of rod-shaped
molecules. One can similarly have nematic-like and smectic-like structures
for disc-shaped molecules as shownin Figure 3. Smectic liquid crystals
can be further divided into different classes dependingon the in-pane order
that leads to smectic phases described by different letters such as smectic
A, smectic B etc. A detailed discussion of these materials can be found in
a book by Gray & Goodby (4).
Electro-Optic Effects
In the rest of this review we focus mainly on the electro-optic properties
of liquid crystals. Since the discoveryof the first liquid crystal, the under-
Smectic
Fiyure 2 Schematic representation of nematic and smectic A liquid crystals with rod-shaped
molecules.
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Nematic
Smectic
Figure3 Schematic
representationof nematicandsmecticAliquid crystals withdisc-shaped
molecules.
standing of these somewhatunusual materials progressed at a snails pace

for almost eighty years. It was not until the discovery of the twisted nematic
effect (5) about twenty years ago that the field really beganto accelerate,
in part due to the financial lure. The primary thrust of liquid crystal device
research and development has been aimed at large area, high information
content displays because of the potentially large market in the form of
consumerelectronics. However,the use of liquid crystals for spccialized
device applications such as optical image processing is an issue that has not
attracted the attention of most manufacturers due to lack of an identifiable
market.
It is perhaps appropriate to first identify someof the general differences
that exist between display devices and spatial light modulators. While the
display devices are generally intended as interfaces between humanand
visual information, the spatial light modulators can be considered as
information processors. Althoughdisplays can also be thought of as spatial
light modulators, these devices ar~ not completely interchangeable. In
Figure 4 we summarizesome of the differences between spatial light modu-
lators and displays. The size constraint on spatial light modulators may
be artificial and maysimply reflect the fact that most optical components
such as lenses are small, and therefore to maximizethe throughput of the
system, the spatial light modulators must also have to be small.
DIELECTRIC ANISOTROPY
The most widely used effect in nematic liquid crystals for electro-optic
devices is the dielectric re-orientation effect. The anisotropy of the liquid
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LIQUID CRYSTALS 273
DISPLAYS SLM
High Prod. Volume LowProd. Volume
LowCost High Cost
LargeViewingAngle SmallWavefrontDistortion
Multiplexable Phaseand Amplitude

Polychromatic - Monochromatic
LargeSize Small Size

Figure 4 Comparisonof spatial light modulatorsand displays.
crystal molecules results in two values of the dielectric constant, one

parallel to the long axis of the molecules (ell) and the other perpendicular
to the long axes (e). Anexternally applied electric field forces the molecules
to reorient such that the axes of the molecules with the largest dielectric
constant lie parallel to the electric field. Amaterial is said to havepositive
dielectric anisotropy if ell > e and negative if ell < el. In somematerials,
however, this distinction becomesunclear because of differences in the
dispersion of the two dielectric constants. This can producepositive dielec-
tric anisotropy at low frequencies and negative anisotropy at high
frequency. Those materials in which the sign of the dielectric anisotropy
changes with frequency are often referred to as two-frequency materials.
The most popular device using this effect is the twisted nematic device
(5), shownin Figure 5. This device consists of two conductively coated
glass plates separated typically by a 10 #mgap in which the liquid crystal
is confined. The inner surfaces of the cell contain an .alignment coating
that is unidirectionally rubbedsuch that the angle of the rubbing direction
on the two surfaces differs by 90. This alignmentlayer forces the molecules
to lie parallel to the rubbing axis thus forming a twisted structure with the
twist axis normal to the surface. Since for the fiematic liquid crystal, the
twist could be right- or left-handed, a chiral dopant is often addedto the
liquid crystal to break this symmetry. Twopolarizers are attached to the
outer surfaces of the cell, with the polarization axis parallel to the rubbing
axis. In the transmission mode, the light passes through the polarizer,
through the liquid crystal, and emerges with a 90 rotation of the polar-
ization. The polarization rotation is due to adiabatic following (6) of the
twisted liquid crystal structure. This modeconstitutes the on state. Note
that complete adiabatic following of the polarization occurs only if the
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274 PATEL
Polarizer
,. Glass ~
Polarizer
OFF ON
Figure 5 Operation of a twisted nematic device.
wavelength of the light is shorter than the helical pitch (7). Whenthis
condition is not satisfied, modemixing occurs and the light that emerges
fromthe liquid crystal is elliptically polarized. In the presenceof an electric
field, the moleculesre-orient parallel to the electric field. This results in
the destruction of the helical structure, whichin turn prevents the rotation
of light through 90. Whenthe light encounters the second polarizer, it is
blocked. This results in the off state.
A complication arises whenthe issue of electrically connecting a large
numberof pixels is considered. For example, consider a matrix of 100 100
pixels. For direct addressing this would require a minimumof 104+ 1
wires; one for each of l0 4 pixels and one commonground electrode. This
can be done more simply by using only 200 wires if matrix addressing is
employed. However, the use of this addressing technique requires the
presence of a threshold voltage below which no switching occurs. Ideally,
the electro-optic response function should be a step function with a non-
zero value. The liquid crystal devices, such as the twisted nematic device,
possess a threshold often referred to as the Fredericks threshold, deter-
mined by the material parameters and the surface conditions such as the
angle that the director makeswith respect to the surfaces. In attempts to
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LIQUID CRYSTALS275
makea bistable nematic liquid crystal cell, Berremandiscovered that the
electro-optic response function could be significantly altered, not only by
controlling the material constants and the surface tilt angle, but also by
varying the amount of twist in a twisted nematic display (8). This led
to various twisted nematic configurations (9). The improvement in the
nonlinear response function results in a matrix display that has morelines
and higher contrast. This can be appreciated by noting that in a matrix
addressing scheme(10), the ratio of the voltage between the selected (Vs)
and non-selected (Vns) element is given
Thus for a 100 x 100 element matrix, there is only a 10%difference in

voltage between the select and nonselect elements. This must produce a
significant contrast between the selected and the nonselected element in
order for this schemeto be employed, which clearly indicates the import-
ance of a steeper electro-optic response function. More recently, com-
mercial products such as portable televisions that have incorporated a
nonlinear response function produced by a transistor are beginning to
appear on the market. Since a transistor is a switch, it can ideally be
considered as an element with infinite nonlinearity, which is limited only
by the leakage currents. While research in this area has been extensive, it
is only recently that active matrix displays of sizes up to 14.5 inches in
diagonal have been made in Japan (11).
FLEXOELECTRIC EFFECT
The flexoelectric effect in liquid crystals was first predicted by Meyer(12).

This effect is similar to the piezoelectric effect in solids (13) in which
mechanical strain in the system results in polarization. The flexoelectric
effect arises primarily because of the geometrical packing constraints
imposed on asymmetrical molecules. Consider, for example, a pear-shaped
molecule that has a dipole momentalong its long axis. If such molecules
are confined in a rectangular box, they will arrange themselves to produce
a net zero macroscopicpolarization. If, however,the container is deformed
as shownin Figure 6, then the packing constraints result in a net non-zero
value of polarization. The magnitude of this polarization would depend
on the amount of curvature and also on the material parameters such as
the magnitude of the dipole moment,and the asymmetryof the object. In
order to quantify this effect, the material properties are grouped into a
single parameter called the flexoelectric coefficient ~s. The subscript s
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276 PATEL
Figure 6 Flexoelectric polarization induced by splay (top right ) and bend (bottom right)
deformations.
simply indicates that the coefficient is related to the amount of splay

deformation. Since it is also possible to have bend deformation, there is
another coefficient Yb associated with this type of deformation. Howthe
macroscopicpolarization is generated by bending the system is illustrated
in the bottom right of Figure 6.
It is the inverse effect that is moreuseful for electro-optic devices because
an externally applied electric field causes structural deformation that can
produce an optical change. An early experiment to measure the flexo-
electric coefficients in nematic liquid crystals can also be considered as a
demonstration of a device capable of arbitrary polarization rotation (14).
The details of the physical cell structure aside, it is seen that the rotation
is caused by changing the amountof twist in the cell by changing the in-
plane DCelectric field. The device is capable of analogue polarization
rotation between -45 and +45. The response is slow, however, since the
device has to be operated at low voltages to avoid interference from the
dielectric anisotropy effect described previously. The polarization rotation
was found to be proportional to the magnitudeof the applied electric field.
The flexoclectric effect in cholesteric liquid crystals results in a linear
electro-optic effect (15). The" helical structure characteristic of a cholesteric
liquid crystal can be modified or even completely unwoundby an applied
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LIQUID CRYSTALS 277

electric field. This is well understoodin terms of the couplingof the electric
field to the dielectric anisotropy of the liquid crystal, an effect that is
quadratic in the amplitude of the electric field. In order to observe the
flexoelectric effect in cholesteric liquid crystals, this dielectric effect should
be suppressed or preferably eliminated. The flexoelectric effect is easily
observedin a well-aligned parallel plate cell in whichthe helix axis of the
cholesteric liquid crystal lies in the plane of the plates. In this configuration,
in the absenceof an electric field, the cholesteric liquid crystal behavesas
a uniaxial material with its optic axis perpendicular to the helix axis. When
an electric field is applied, the helix distorts, as shownin Figure 7, to lower

the free energyof the system(14). Thenet result of an applied electric field
is that the system behaves as if the optic axis had been rotated about the
electric field direction. The direction and the magnitudeof this rotation is
proportional to the direction and the magnitudeof the applied electric field.
Thus this effect is a linear electro-optic effect and phenomenologically
resemblesthe ferroelectric effect and the electroclinic effect in liquid crystals
that are discussed below.
The fact that the optic axis of the liquid crystal can be influenced by the
applied electric field indicates that this effect can be used to produce an
electro-optic modulator. This can be seen clearly by noting that the
transmission of light through a structure consisting of a birefringent medium
placed between two crossed polarizers, such that the optic axis of the
birefringent mediumforms an angle fl with respect to the polarizer axis,
is given by
I = I0 sin2 (2fl) sin2 (~b/2). 2.
E<O E=O E>O
Figure 7 Cholcsteric helix distortion causedby flexoelectric effect.

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278 PATEL
Here ~b = 27tAnd/2, the phase shift through the sample, where An denotes
the birefringence, 2 the wavelength of the light in vacuum, and d the
thickness of the sample. Thus whenan applied electric field is modulated,
it produces a change in /~ that translates into an intensity modula-
tion. Therefore for an alternating electric field, the angle changes as
(/~ +__ ~) resulting from the helix rotation, which causes intensity modula-
tion, and
AI/I" tan (2/~) = sin (4~). 3.
It can be shownthat tan = eE/toK ~ for small angles, where e is the

flexoelectric coefficient (11), K is the elastic constant, 2Z/to is the helical

pitch, and E is the electric field. This linear relationship between the
magnitudeof the applied electric field and the helix rotation angle is shown
in Figure 8. Figure 9 shows the optical response to an applied square wave
to illustrate the speed of this switching. The intensity has been normalized
to comparethe rise and the fall time at different voltages. The switching
speed is of the order of 100/~sec. Furthermore, by comparingthe switching
speed for two different voltages, it is found that the times are independent
of the applied electric field (16) although the absolute electro-optic effect
is proportional to the magnitudeof the field. The rise and fall times are
equal as expected because the switching is field-driven for both states. The
field independence of the switching time can be explained by noting that
the torque on the molecules is proportional to the field, but the molecules
0 24 48
Voltage
Figure 8 Rotation of optic axis vs applied electric field.
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LIQUID CRYSTALS 279
0 1000 o .... ooo.... ooo

Time(psec)
Figure 9 Optical response to an applied electric field. The intensity is normalized for
comparison.
have to swing through an angle ~, which is also proportional to the field.

Thus for small values orE, the switching speed is field-independent because
of the compensating effects of the greater torque and larger optic axis
rotation. This can rigorously be shownto be true as long as the linear
relationship holds (17). The measured temperature dependence of this
effect has been found to be weak(18).
FERROELECTRIC EFFECT
Aneffect that has recently received a great deal of attention is the ferro-
electric effect. This was first predicted and experimentallyverified by Meyer
(19), whoshowedthat a tilted smectic liquid crystal composedof chiral
molecules can possess ferroelectric properties because of the reduced sym-
metry of such a system (20). Clearly all tilted smectic phases, of which
there are several, are capable of exhibiting ferroelectric properties provided
the molecules are chiral. In what follows, we primarily limit ourselves to
smectic C* phase, which has the least in-plane order, and hence is the
fastest switching.
In a smectic C* phase, the chiral nature of the molecules produces a
helical structure (Figure 10a) such that the molecules in successive layers
are slightly more twisted than the preceding layer (21, 22). The polariz-
ation, which lies in the layer plane and perpendicular to the long axis of
the molecule, also follows a helicoidal path, and thus the macroscopic
polarization vanishes because of compensating momentsin a thick sample.
Clark &Lagerwall have shownthat it is possible to operate a ferroelectric
liquid crystal device in a bistable manner(23) if the helicoidal twist of the
ferroelectric smectic phase is suppressed by surface forces (Figure 10b).
The cell thickness must be less than the pitch of the material (24). Under
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280 PATEL
(a) TopView
I
I r.icCell
I
f surfaceStabilized
Helix Unwinding
~ ~ Thin Cell
(c) ~ElectricField
~ ~ ] Dark View
,~ J ~ Bright View
(e) ~ Field Turned

off
FiyureI0 (a) Helicalstructureof smecticC*,(b) surfacestabilizedstructure,(c) effect

appliedandelectric field, (d) effectof reversingthe electricfield direction,(e) effect
removingthe electric field (figure adaptedfromKondo K., ct al. 1983.Jpn.J. Appl.Phys.
L85:22).
these conditions, the director is confined to a horizontal surface and only

two orientations are possible. The sample, therefore, consists of two types
of domainsthat are separated by domainwalls. The polarization direction
in the two domainsis opposite to each other. Henceby applying an electric
field, one of the domainscan be increased in size while decreasing the size
of the other. This effect can be used to produce gray levels by space
division. While this effect has been known(25) for some time, Hoffman
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LIQUID CRYSTALS 281
recently showedthat it can be controlled quite precisely by controlling the

amountof charge supplied to a given pixel (26). By reversing the field, the
phenomenoncan be reversed (Figure 10d). If the field is removedat this
stage, a memory effect is observed due to the bistable nature of the device
(Figure 10e). Since the optic axis in the two domainslies at different angles,
optical modulation can be achieved by placing such a device between
polarizers such that the optic axis of one of the states lies parallel to the
polarizer axis (see left-hand side of Figure 10). The angle between the
optic axis in the two states changes with temperature, but with materials
engineering, it can be madeto be equal to 45 at roomtemperature in the

field-driven state. Althoughthe device is bistable, the angle changes to a

smaller value than expected because of the chevron layer structure (27-
29). Thus the measured value of the tilt angle depends on the magnitude
of the applied field presumablybecause of layer distortion (30). Recently
it was shownthat the chevron layer structure can be reversibly eliminated
at a threshold field (31). Our recent work (32) shows that this structure
can be non-reversibly removed by using a large ACfield. However, in
doing so, the bistability is also lost since the layer rearrangement also
causes layer reorientation such that the optic axis of one of the states lies
parallel to the buffing axis. The advantage of this layer reorientation is
that the full optic angle is recovered, thus allowing higher contrast between
the on and off states. The switching speed of these devices continues to
improveand is at the present of the order of 20 #sec at an applied field of
15 V//~m.
Werecently demonstrated a new ferroelectric liquid crystal structure
that combines the fast speed of a ferroelectric and the optical behavior
of the twisted nematic structures (33). This ferroelectric twisted smectic
structure (FETSS)allows fast switching and, at the same time, variable
transmission. The structure is described in Figure 11, which is obtained
by rubbing the cell surfaces at an angle of 90 with respect to each other.
In this case, a mono-domainsample is obtained, with the smectic layers
forming at 45 to the rubbing axis. The smectic layers are arranged so that
the layer normalis parallel to the glass surface, in the so-called bookshelf
geometry. Within each layer, the projection of the molecules on the cell
surface rotates by 90 in going from one surface to the next. The molecules
must be tilted by an angle equal to the tilt angle with respect to the layer
normal since it is an order parameter of the smectic liquid crystal. Thus
the moleculeslie in the plane of the substrate at the cell surfaces, but they
deviate from this plane in the middle of the cell. Figure 11 schematically
shows that the molecules are constrained to lie on the surface of a cone.
The local ferroelectric polarization /~ of this sample undergoes a 180
rotation in going from one surface to the other. This is because the polar-
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282 PATEL
(a) (b)
Fi#ure11 Representation
of ferroelectrictwistedsmecticstructure.
ization direction is constrained to lie in the plane of the smectic layers and
normal to ~i. This coupling between a and/~ is important because it allows
the molecular position to be changed by reorienting/5 using an externally
applied electric field.
Optically the twisted smectic structure would appear similar to the
twisted nematic structure. This is because the optical eigen modes of
this sample are also linearly polarized whenadiabatic following occurs.
Therefore, linearly polarized light passing through such a structure is
rotated by an angle equal to the twist in the structure. The incominglight
passes through a twisted smectic when a sample is placed between cross
polarizers such that the rubbing axes at the two surfaces coincide with the
polarizer axes. Onthe other hand, whenthe electric polarization lines up
with the direction of the applied field, it forces the moleculesto be parallel
to each other. This destroys the twisted structure and therefore the light
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LIQUID CRYSTALS 283
does not get through. Note that if the molecules at the two surfaces are to
remain parallel to the rubbing axis (using strong anchoring), then there
wouldbe an abrupt change in the molecular orientation close to the surface
as shownin Figure 11. These two optical states are the limits. It is also
possible to unwindthe twisted structure slightly by applying a smaller
electric field. In this intermediate case, the optical eigen modesof the
ferroelectric liquid crystal structure are elliptical and, therefore, only part
of the initially polarized light will get throughthe structure. In this wayit
is possible to obtain continuously variable transmission as shownin Figure
12.
ELECTROCLINIC EFFECT
Aneffect similar to the ferroelectric effect in liquid crystals is the electro-
clinic effect, which was discovered by Garoff &Meyer(34) in 1977. This
effect is observed in smectic A and other orthogonal phases (35), such
smectic B and smectic E composedof chiral molecules. In these phases,
the layers develop perpendicular to the long axis of the molecules, and the
application of an electric field causes the molecules to reorient about the
field axis such that there is an effective moleculartilt with respect to the
0.4
0.2 ./ i
-2.0 -1.0 0.0 1.0 2.0

Volts
Fi#ure 12 Gray scale capability of the modulator by applying randomly varying voltages.
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284 PATEL
layer normal. In order to understand the origin of this effect, consider
the ferroelectric smectic C* phase in which the molecules give rise to a
spontaneous polarization. This polarization arises only because of reduced
symmetry(C2) of the system and vanishes when the tilt angle is reduced
to zero because the symmetry changes to (C~), which indicates that the
polarization and the tilt angle are fundamentally related. With this cou-
pling in mind, the electroclinic effect is caused by an induced polarization
(produced by an externally applied electric field) that produces a molecular
tilt in the system. Its magnitudedepends on the degree of coupling between
the polarization and the molecular tilt. The coupling coefficient between
polarization and the moleculartilt is called the electroclinic coefficient. Its

magnitude depends on the chemical makeupof the liquid crystal molecules
as well as the intermolecular interactions. Clearly those molecules that are
likely to produce a large polarization in the ferroelectric smectic C* phase
will have a larger electroclinic effect. Thesecorrelations have recently been
established (36). Recentlythe increased interest in the field of ferroelectric
liquid crystals has produced materials with large spontaneous polarization
in the smectic C* phasc that also possess a smectic A phase, which has
provento have a large electroclinic effect. It is these recent developments
in materials that mayhave madethis effect of practical value. While one
mayexpect that the magnitudeof the effect is linear in an electric field,
which it is at small fields and at temperatures far from the smcctic A to
smectic C* phase transition, it becomesnonlinear at high fields and at
temperatures close to the phase transition. The effect is also temperature-
dependent and is maximum close to the phase transition (35, 36). Figure
13a showsthe relationship betweenthe tilt angle and the applied electric
field at various temperatures in the vicinity of the smectic A to smectic C*
phase transition. As long as the linear relationship between induced tilt
angle and the applied electric field holds (37, 38), the switching speed
expected to be independent of the applied electric field. The experimental
results are shownin Figure 13b.
COMPARISON OF POLAR EFFECTS
A comparison between the advantages and the disadvantages of each of

the polar effects described aboveis summarizedin Figure 14. In the figure,
the flcxoelectric columnrefers to the cholesteric liquid crystal device using
this effect. Theferroelectric refers to the surface-stabilized thin cell device,
whereasthe electroclinic refers to the electric field effect in the smectic A
phase. The switching times are estimated based on reported values of
this parameter. Clearly this is not a straightforward variable because the
switching speed depends on the magnitudeof the applied field, at least in
Annual Reviews
LIQUIDCRYSTALS 285
25.0 A 50.0
20,0 ~P" 40.0

..
5.o 30.0:
~o.o. ~* .~ ~,~ a 20.0
5.0 ~ ~o.o
0.0 - ........ 0.0

0.0 8.0 16.0 24.0 32.0 40.0 0.0 3.0 6.0 9.0
ELECTRIC FIELD (V/~m) ELECTRIC FIELD(V/~m)
Figurel 3 (Left) Changeof tilt angle with electric fleld, (right) switching speed as a function
of applied electric field. The four curves represent data 2, 4, 6, and 8 below the phase
transition temperature.
the case of the ferroelectric effect. Furthermore, the temperature of the

sample and the nature of the liquid crystal also influence the switching
speed at a fixed applied field. Similarly, because these materials are aniso-
tropic, viscosity is a tensor quantity and therefore cannot be easily
compared. This problem becomes even more complicated by the fact that
different components of the tensor comeinto play for these different effects.
In spite of these parameters, some effective value of viscosity can be
assigned if the applied torque and the switching time are known. It is
expected that the smectics that are more ordered have somewhathigher
viscosity than the cholesteric, although this assumption should be viewed
with caution. Clearly the linear electro-optic effects, such as the flexo-
electric and the electroclinic effects do not possess a voltage threshold as
is required for matrix addressing as described above. Ferroelectrics, on
PARAMETER FLEXOELECTRI(~ FERROELECTRIC ~
TIME 1 msec- 100~sec 1 msec

o 10 pse 0.1 msec-0.1 psec
TILT ANGLE linearIn E constant linearIn E

THRESHOLD none Vx t none
VISCOSITY small large large
TEMPDEPEN small large severe

TEMPRANGE large large verysmall
Figure 14 Comparisonof various polar electro-optic effects.
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286 PATEL
the other hand, do possess a dynamicthreshold that dependson voltage
and duration of time for whichthe voltage is left on. Thusa short high
voltage pulse mayswitch the samplejust as well as a long low voltage
pulse, although the response time wouldbe different. It has been shown,
for example,that the threshold voltage dependson the product of the
applied pulse-width and the voltage, although deviations from this
relationship are observed for more complexwaveforms(39). Whilethe
flexoelectric effect showsa very small temperaturedependence,the ferro-
electric shows a great amountof temperature dependence primarily
becauseof the changingtilt angle. Theelectroclinic effect showsthe most

severe temperature dependence,whichmakesits operating temperature

range somewhatlimited.
STRUCTURE-PROPERTY RELATIONSHIPS
Considerableprogress has been madein developingnewchiral smectic C*

materials for ferroelectric liquid crystal displays. Materials for nematic
liquid crystals are reasonably well understood, although muchwork is
being done to improvethe performanceof these materials for commercial
applications.Wefirst considerbriefly the aspectsof the molecularstructure
that can be changedto producethe desiredproperties. It shouldbe stressed,
however, that although trends can be identified in this manner,these
structures are complex,and the effect of a single molecularchangemayin
fact havedramatic effects on macroscopicphysical properties.
Nematics
Thenumberof identified nematicliquid crystals is enormous.Thestructure
can roughlybe dividedinto three segments.Theuppertail, the body,often
called the core, andthe lowertail. Thetails generallyconsist of a flexible
hydrocarbon,while the core maycontain one or morebenzenerings, which
maybe fused and linked with various functional groups. Consider, for
example,a simple structure linked by a carbonylgroup. It can be achieved
in two ways: either (CO)Oor O(CO).These two structures can and
often do havedrastically different propertiesfor reasonsthat are at present
unclear. A single series of compounds can be generated by changingthe
tail lengths and the bodystructure. For example,a chain length ranging
from 2 through 12 produces 100 different compoundsfor a single core
structure. There are thousands of different cores that are possible by
changingthe order of the benzene,naphthalene,or biphenyl-like structures
and the numerouslinking groups. All this easily results in hundredsof
thousandsof liquid crystalline materials. However,a material maynot
haveall the desirableproperties. Fortunatelyall the nematicliquid crystals
Annual Reviews
LIQUID CRYSTALS 287
are completely miscible with each other. This allows for easy blending of
various liquid crystals to produce the properties desired. The different
liquid crystal devices require that different physical properties of the
materials be optimized. Consider the twisted nematic device as the
example. This device, below the Fredericks threshold voltage, does not
showany optical change. This is an important requirement for an ordinary
multiplexed display. The sharpness of this threshold is determined by the
ratio of the splay and the bend elastic constants (K~/K3), which assumes
infinite anchoring. Theseelastic constants can be altered to a limited extent
by changing the compositionof the materials. This ratio should be typically

greater than 1 and is favored by compoundshaving long alkyl chains (40).

The presence of branched alkyl chains, on the other hand, tends to destroy
the nematic phases and favors smectic phases (41). The magnitude of the
dielectric torque dependsnot only on the magnitudeof the field, but also
on the dielectric anisotropy. The dielectric anisotropy is greater in the more
ordered nematic (characterized by the order parameter) and composed
molecules that are more polar. However,increasing the polarity often can
result in anti-parallel ordering of the dipoles that tends to decrease the
dielectric anisotropy. The other parameter of importance is the viscosity
of the materials. This should be as small as possible. Recent materials
trends have been to decrease the viscosity by introducing fluorine in the
structures of the molecules (42), on the other hand, lateral substitution
tends to increase the viscosity.
Ferroelectrics
Progress in the synthesis of newferroelectric materials has been tremen-
dous in the last ten years in part because of the need for new materials
that operate at room temperature and have the desired fast switching
properties. The trend has been to alter one of two properties, the magnitude
of the polarization, or the magnitudeof the viscosity. Whilelarger polar-
ization allows for larger torque, this is not always a desirable property,
particularly whenrapid switching is desired. This is because during the
switching process, a large amountof charge has to be deposited across the
cell in order to first neutralize the existing charge and then to reorient the
polarization. This process requires a large transient current that maynot
be permitted by the resistance of the current-carrying electrodes. This
simply means that the speed would be limited by the layout of the
electrodes, rather than by the magnitudeof the polarization. Furthermore,
the larger polarization mayincrease the viscosity, possibly because of
dipolar coupling, which would make the device slower. Although these
device issues are not always the driving force for new materials research,
they can produce discoveries like the anti-ferroelectric behavior or a new
Annual Reviews
288 ~
class of liquid crystals, the TGBphase (43-45). Through systematic
materials research we nowhave a better understanding of the correlation
between molecular structure and the magnitude of the polarization. For
ex~tmple, the major contribution to the polarization is proportional to the
dipole momentassociated with a chiral center in the molecule (46). The
position of the dipole momentwith respect to the core is also important.
If it is farther from the core, the dipole momentbecomessmaller because
of the greater degree of rotational freedom. Similarly, for a chosen chiral
center position with respect to the core, if the tail length is increased, the
polarization increases because of the reduced degree of freedom of the
chiral group (47). The observation of an unusual temperature dependence

of the polarization has led to the conclusion that the different conformers
of the molecule can compete to produce the observed polarization (48).
similar effect has also been observed for induced polarization, which is
important for the electroelinic effect (49). Materials with large polarization
usually have a very small helical pitch in the smectic C phase (50). Our
early observation (51) of such materials had shown that they do not
undergo polarization reversal as do the conventional low polarization
materials. For example, during polarization reversal (52), several current
peaks were observed when only one should be expected. To explain this,
several different factors have to be taken into account. Amongthese are
the possibility that the sample may or maynot have a helical structure
because of surface stabilization and that the polarization reversal can
occur at different voltages for the bulk and for the surfaces. Consider, for
example, the simple polarization reversal in a surface-stabilized structure.
Clearly in this case the process of polarization reversal would require
current flow in the external circuit to compensatefor charge on the cell.
Thus a charge of 2Qis required to reorient the sample that is initially in
one state. This can be understood by realizing that an amount of charge
Q is required to first neutralize the existing charge on the cell and an
additional amount of charge Q is needed to polarize the structure in the
opposite state. These two artificially separated processes can occur
simultaneously, and only one current peak is observed during polarization
reversal for somematerials. This, however, maynot be the case for samples
that have a helical structure. Here the polarization reversal can actually
take place in two stages, the first requiring charge Q to produce a wound
state from an initially unwoundstate, and the second requiring an addition
of charge Q to polarize the structure in the opposite state by unwinding
of the woundstate. If the sample is completely woundin between the two
electrically unwoundstates, the charge associated with the two current
peaks wouldbe exactly the same, otherwise it would be different. Further-
more the separation between the peaks would depend on the frequency of
Annual Reviews
LIQUID CRYSTALS 289
the applied electric field and the rate at which the sample winds up
elasticity. The electric field value for the temporal position of the first
current peak can be calculated by balancing the field energy against the
twist elastic energy and is given by Ec = ~2Kq~/Ps.Morecurrent peak can
occur if the bulk and the surface molecular reorientation occur at different
field value. Thus in a tightly woundsample it is possible to observe
four distinct events. In our early investigations of materials with high
polarization and tight pitch, four peaks have indeed been observed. The
unambiguousidentification of these events as described above, however,
was not made. The interpretation of the data was further complicated by
the discovery of the possible antiferroelectric ordering in the materials

similar to the ones that we had examined.It is worth considering this model
for a moment.In the proposed modelof the antiferroelectric ordering, the
successive layers have a moleculartilt in opposite directions, but a pair of
these layers still retains the helical structure (53). Let us examinewhat
might happen to such a sample when subjected to a triangular wave
voltage, which changes sign from - V to V periodically. At high enough
negative voltages, the sample would be completely unwoundwith a charge
on the cell equal to - Q. Slowly decreasing the voltage wouldresult in the
occurrence of one of two processes. In one, the material would undergo
antiferroelectric pairing at a well-defined voltage determinedby the pairing
energy, which wouldrequire the deposition of charge Q to compensatefor
the charge on the cell. This critical voltage woulddependon the thickness
of the cell since the critical voltage, in this case, is simply determinedby
the equation P" V/d = Vim , where Vin t is the pairing interaction energy. In
the other case, the sample first winds up, but no antiferroelectric pairing
occurs. In this case the onset of the current peak wouldhappen when the
field energy becomesless than the elastic energy, as described above. In
the first example, the antiferroelectric pairing is followed by the winding
of the helix, but since the charge on the cell is zero, no additional current
peak would be observed. Similarly in the second case, the winding up
process can be followed by the antiferroelectric pairing, and this also does
not produce any current peaks. Oncethe voltage across the cell changes
sign, however, another current peak would be observed that results from
exactly the opposite process. In this discussion we have assumedthat the
wholecell switches uniformly in the bulk and at the surfaces, but dropping
this assumption complicates the interpretation even more. Since two peaks
can be observed during voltage reversal due to two different processes, it
is difficult to unambiguouslyprovide evidence of antiferroelectric pairing
from electrical studies alone. There are reports in the literature, however,
where authors have interpreted the occurrence of two current peaks in
switching studies as evidence of antiferroelectric behavior.
Annual Reviews
290 PATEL
ALIGNMENT
One of the more active areas of research has been the search for new
alignment techniques (54) and the study of anchoring effects (55).
fascination with this area of research has been perhaps because of the
almost magical properties of rubbed surfaces to orient liquid crystals in
the direction of rubbing. There are several different types of alignments
depending on the desired orientation of the molecules at the surfaces. The
two commontypes of orientation are the planar or the homogeneous
alignment, in whichthe molecules lie in the plane of the substrate. In the
other type, called the homeotropic alignment, the molecules lie per-
pendicular to the surface plane. There continues to be somedebate about

the mechanism responsible for this alignment. It is perhaps now clear
that for the case of planar alignment there are at least two responsible
mechanisms. These mechanisms depend on the nature of the alignment
coating deposited on the surface prior to rubbing. In one case, the
deposited materials are hard and often cross-linked. Here the alignment is
most probably due to micro scratches that are produced during the rubbing
process. The liquid crystal orientation with respect to the scratches is such
that the molecules would have to prevent splay and bend deformations
that would result in a higher free energy for the system. This has been
quantified by Berreman, whohas shownthat the excess free energy depends
on the shape of the grooves, their separation, and their depth (56, 57).
Specifically, the free energy difference increases with smaller distances
between the scratches or grooves, with deeper grooves, and with the sharp-
ness of the edges. The other mechanismis primarily for the softer materials
like straight chain polymers, such as nylons and polyesters, that can be
stretched in the bulk form. These materials, when rubbed, do not show
much evidence of grooves or scratches when viewed with a scanning
electron microscope (58). However, they often show alignment properties
that are far superior to those of hard materials such as cross-linked poly-
imides (59). This can be illustrated by the observation that while both these
surfaces produce quite good alignment for nematic materials, only the
softer polymer materials are able to align smectic materials. The mech-
anism of alignment in the case of the polymers is the polymer chain
reorientation during the process of rubbing. The evidence for chain orien-
tation is obtained by measuring the small birefringence resulting from this
process (60).
There also exist other methodsof alignment such as oblique evaporation
of inorganic materials, for example SiO2, which was first demonstrated
by Janning (61), although mono-domain samples were obtained much
earlier (62, 63). Numerouspublications showthe use of a wide variety
Annual Reviews
LIQUID CRYSTALS291
materials for alignment; however, the principle is essentially the same.
There have been more complex techniques of alignment involving multiple
evaporationof SiO ~ at different angles to control the surface tilt angle that
the director makeswith the surface (64). In conventional SiO2 evaporation,
the surface tilt angle depends on the direction of the evaporation and, to
a certain degree, on the liquid crystal as well. Furthermore, the direction
of the director in the plane of the substrate is collinear with the direction
of the evaporation. However,at higher angles of evaporation, a curious
change in this direction occurs such that the direction of the director in
the plane of the substrate becomes perpendicular to the angle of the
evaporation. Recently, by careful control of the direction of the angle of

evaporation and the thickness of the evaporated materials, researchers
have found that the surface can exhibit bistable orientation of the director
in a narrow region of evaporation angles and the deposited material
thickness (65). They have used these surfaces to produce bistable nematic
liquid crystal devices (66).
There has been some research in producing photo-active surfaces for
controlling the molecular alignmentby light. This is an interesting concept
that allows one light beamto control another. Furthermore, a small change
in the surface properties can influence a large numberof liquid crystal
molecules, which results in amplification of the optical effect, e.g. the
alignment layer of 300 A controls the molecular orientation of a 10 #
thick cell. This produces an optical amplification of over 300. It has been
reported, for example, that azo groups containing alignment materials can
be used to change molecular orientation from homeotropic to homo-
geneous alignment and vice versa (see Figure 15) by illuminating the
alignment layer with radiation of 365 or 440 nm, respectively (67). Azo
group-containing materials have also been deposited in the form of Lang-
muir-Blodgett films as photochemical alignment layers (68). The mech-
anism of this alignment change is due to the conformational change that
the azo group undergoes under the action of light. Photo-active surfaces
o.Oooo.o
ooooo Molecules
o,
U Oi u uou
o,,o,o
,o
Figure15Photochemically
inducedreversiblechangeof liquid crystal all.merit (adapted
fromReference
65).
Annual Reviews
292 PATEL
have also been used to control orientational behavior using the polar-
ization of light to reorient the liquid crystal direction from one homo-
geneous orientation to another (69). The authors reported that nematic
liquid crystals in an illuminated region becomeoriented perpendicularto
the direction of the electric-field polarization of the light and remain
aligned in the absenceof the radiation. The fact that the alignmentremains
after light is removedindicates that it is the photo-activesurface that is
responsible for molecularalignment. The alignmentin the surface layer as
a result of light can be traced back at least to the workof Todorovet al
(70), which suggests that the dye-doped polymeris oriented because

anisotropic absorption of the dye molecules that undergomolecular re-

orientation of re-arrangementwhich in turn orients the polymer. Similar
dye-dopedmaterials have becn used recently as optical recording materials
(71).
CONCLUSIONS
The various liquid crystal effects combinedwith a wide variety of liquid

crystal types, in a broadrangeof possible materials, allow great flexibility
in designing displays and spatial light modulators. Progress in the dis-
covery of neweffects and newmaterials is certain to further broadenthe
pool of available displays and spatial light modulatorsin areas such as
communications.
ACKNOWLEDGMENTS
I would like to thank my collaborators, Sin-Doo Lee and J. W. Goodby

for their participation in someof the research projects described in this
paper.
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Annual Reviews

Annu. Rev. Mater. Sci. 1993. 23:269-94

LIQUID CRYSTALS: Materials for

KEYWORDS: nematics,snaectic, electro-optic,ferroelectric effect, flexoelectric

revealed by using a polarizing microscope. These materials also share

properties of liquids in that they are fluids. The commonnematic liquid

LIQUID CRYSTALS 271

Wcfocus on matcrials with rod-shaped molcculcs, which can bc sub-

standing of these somewhatunusual materials progressed at a snails pace

LIQUID CRYSTALS 273

High Prod. Volume LowProd. Volume

LowCost High Cost

Multiplexable Phaseand Amplitude

LargeSize Small Size

crystal molecules results in two values of the dielectric constant, one

Thus for a 100 x 100 element matrix, there is only a 10%difference in

The flexoelectric effect in liquid crystals was first predicted by Meyer(12).

simply indicates that the coefficient is related to the amount of splay

LIQUID CRYSTALS 277

an electric field is applied, the helix distorts, as shownin Figure 7, to lower

E<O E=O E>O

Figure 7 Cholcsteric helix distortion causedby flexoelectric effect.

It can be shownthat tan = eE/toK ~ for small angles, where e is the

flexoelectric coefficient (11), K is the elastic constant, 2Z/to is the helical

LIQUID CRYSTALS 279

0 1000 o .... ooo.... ooo

have to swing through an angle ~, which is also proportional to the field.

(e) ~ Field Turned

FiyureI0 (a) Helicalstructureof smecticC*,(b) surfacestabilizedstructure,(c) effect

these conditions, the director is confined to a horizontal surface and only

LIQUID CRYSTALS 281

recently showedthat it can be controlled quite precisely by controlling the

engineering, it can be madeto be equal to 45 at roomtemperature in the

field-driven state. Althoughthe device is bistable, the angle changes to a

LIQUID CRYSTALS 283

-2.0 -1.0 0.0 1.0 2.0

polarization and the moleculartilt is called the electroclinic coefficient. Its

COMPARISON OF POLAR EFFECTS

A comparison between the advantages and the disadvantages of each of

20,0 ~P" 40.0

0.0 - ........ 0.0

the case of the ferroelectric effect. Furthermore, the temperature of the

PARAMETER FLEXOELECTRI(~ FERROELECTRIC ~

TIME 1 msec- 100~sec 1 msec

TILT ANGLE linearIn E constant linearIn E

VISCOSITY small large large

TEMPDEPEN small large severe

becauseof the changingtilt angle. Theelectroclinic effect showsthe most

severe temperature dependence,whichmakesits operating temperature

Considerableprogress has been madein developingnewchiral smectic C*

LIQUID CRYSTALS 287

by changing the compositionof the materials. This ratio should be typically

greater than 1 and is favored by compoundshaving long alkyl chains (40).

chiral group (47). The observation of an unusual temperature dependence

LIQUID CRYSTALS 289

the discovery of the possible antiferroelectric ordering in the materials

pendicular to the surface plane. There continues to be somedebate about

evaporation. Recently, by careful control of the direction of the angle of

(70), which suggests that the dye-doped polymeris oriented because

anisotropic absorption of the dye molecules that undergomolecular re-

The various liquid crystal effects combinedwith a wide variety of liquid

I would like to thank my collaborators, Sin-Doo Lee and J. W. Goodby

LIQUID CRYSTALS 293