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ELECTROOPTIC DEVICES

The electrooptic effect, which is the change in refractive index with an external
applied electric field, is manifested in certain materials which show tremendous
promise of applications such as light valves, beam deflectors, and optical displays
for optical communications, in conjunction with solid state laser chips and optical
fibers. Compared with liquid crystal devices, the ceramic electrooptic components,
in general, possess advantages in terms of their response speed (µsec), particularly
in falling time, contrast ratio (10 2) and gray scale (16 scales), and their ability to
withstand high intensity illumination. On the other hand, the present ceramic
components require relatively high drive voltages (1 kV) and production cost
($100). Therefore, the development of a simple mass-production process, electrode
configurations with a narrow gap, and improvement of material properties, will be
key factors in the actual commercialization of ceramic optical components.

8.1 ELECTROOPTIC EFFECT - REVIEW

Let us initially review the operation of a light shutter based on the second-order
electrooptic effect (Kerr effect). Birefringence ∆n is induced in a crystal of the
appropriate type when an electric field E is applied, according to:

∆n = - (1/2) R n 3 E2, (8.1)

where R is the quadratic electrooptic coefficient and n is the original refractive


index of the crystal. When this sample is placed between crossed polarizers
arranged at the 45o direction with respect to the E direction, and light is transmitted
through the system as shown in Fig. 8.1, the output light intensity is represented by

I = I 0 A sin 2 [(π R n 3 L / 2 λ) E2 ], (8.2)

where I0 is the incident light intensity, A is an equipment constant, L is the path


length (i.e., the sample thickness), and λ is the wavelength of the light. The voltage
required for the first intensity maximum is an essential device parameter called the
half wave voltage.

221
222 Chapter 8

Polarizer Analyzer

45 o - 45 o
L

PLZT

Electric field

Fig. 8.1 Fundamental construction of an electrooptic light shutter.

8.2 TRANSPARENT ELECTROOPTIC CERAMICS


Since the 1960s the non-linear polarizability of ferroelectrics has been investigated
rather extensively, and various electrooptic and optical parametric devices have
been developed. However, problems still remain in preparing high grade optically-
homogeneous single crystals and, hence, manufacturing costs are generally high.

The polycrystalline microstructure of a ferroelectric ceramic can also exhibit the


electrooptic effect if it is sintered to a pore-free state to make it transparent. Relaxor
ferroelectrics are of special interest for non-linear optic applications because an
extraordinarily large apparent electrooptic Kerr effect can be observed even when
the material is in its so-called paraelectric state. This section describes the
fundamental electrooptic properties of perovskite-type polycrystalline and single
crystal ferroelectrics.

(1) (Pb,La)(Zr,Ti)O3

The most useful ferroelectric electrooptic materials have traditionally come from the
(Pb,La)(Zr,Ti)O3 system; they generally have good transparency in a wavelength
range extending from the visible to infrared, and exhibit optical anisotropy with an
applied electric voltage. Figure 8.2 shows the phase diagram of the (Pb 1-xLa x)(Zr 1-
y Tiy )1-x/4O 3 system, on which is indicated the electrooptic effects manifested for
various phase regions. Notice that the valence of lanthanum ion (3+) in the a-site
(2+) generates the vacancy of the b-site.

The PLZT solid solution exhibits both the Pockels (primary) and Kerr (secondary)
electrooptic effects, depending on the composition. Some examples of typical ∆n
vs. E curves are shown in Fig. 8.3. The electrooptic coefficients of the PLZT
system are much larger than the values in conventional crystals such as LiNbO3 and
(Sr,Br)Nb 2 O6 (SBN) (see Table 8.1), which means that the voltage required for the
electrooptic shutter is much less for the PLZT.
Electrooptic Devices 223

Fig. 8.2 Relation between PLZT compostion and structure and electrooptic
application.

Fig. 8.3 Polarization P and birefringence ∆n as a function of electric field E for


some PLZT ceramics.
224 Chapter 8

Table 8.1 Pockels (1st) and Kerr (2nd) electrooptic coefficients for various
materials.
_______________________________________________________________
Material r (x10-10 m/V)
_______________________________________________________________
LiNbO3 0.17
Ba2(K0.9Na0.1)Nb5O15 0.52
Primary electrooptic KH2PO4 0.52
coefficient (Sr 0.5Ba0.5)Nb2O6 2.10
PLZT 8/65/35 (GS=10µm) 5.23
PLZT 8/65/35 (GS=3µm) 6.12
_______________________________________________________________
R (x10-16 m2 /V2)
_______________________________________________________________
KTa0.65Nb0.35O3 5.30
Secondary electrooptic PLZT 9/65/35 (GS=2µm) 9.12
coefficient PLZT 10/65/35 (GS=2µm) 1.07
_______________________________________________________________

Fig. 8.4 Grain size dependence of the electrooptic coefficients, R and g, for PLZT
9/65/35.

Among the various PLZT compositions, 9/65/35 near the triple point between the
tetragonal, rhombohedral and cubic phases is of particular interest because it
exhibits a large electooptic effect (R = 9.1 x 10-16 m2 V-2 ) and is thus applicable for
light shutters and optical displays.

However, care must be taken to control grain size. Figure 8.4 shows the grain size
dependence of the electrooptic coefficients, R and g (defined as ∆n = - (1/2)g n3 P2 ),
Electrooptic Devices 225

for PLZT 9/65/35.1) The samples were prepared by hot-press sintering starting from
coprecipitated PLZT powders. The electrooptic response is drastically decreased
for samples with grain sizes below 2 µm, which corresponds approximately to the
critical grain size below which the sample loses ferroelectric properties (maybe
antiferroelectric state).2) Therefore, relatively large grain size is necessary to
produce a reasonable electrooptic effect. On the other hand, a significant decrease
in fracture toughness or durability occurs for particularly large grain size samples,
probably due to the B-site vacancies in the crystal structure. A normally sintered
transparent PLZT ceramic, with an average grain size of more than 6 µm, has a
fracture toughness (mode I for tensile stress) of KIC =0.9 MNm-3/2, which
corresponds roughly to durability for 108 cycles of repeated operation.2) This
translates to about only 2 months when the PLZT is used for an image display (TV)
driven at 30Hz.

Example Problem 8.1_________________________________________________

PLZT 10/65/35, with a cubic symmetry shows an electrooptic coefficient (R11 -


R12 ) of 1.1 x 10 -16 [m2/ V2] and n0 = 2.49. Calculate the half wave electric field
for a sample with L = 1 mm, when λ = 633 nm light is transmitted perpendicular to
the electric field. Refer to Fig. 8.1.

Hint

The half wave voltage is calculated from

Γy = (p/λ) n 0 3 E3 2 (R 11 - R12 ) L
= π. (P8.1.1)

Solution

E3 = (λ / n 0 3 (R 11 - R12) L) 1/2
= (633 x 10-9 / 2.493 x 1.1 x 10 -16 x 1 x 10-3) 1/2
= 6.1 x 10 5 [V/m] . (P8.1.2)
___________________________________________________________________

(2) Pb(Zn1/3 Nb2/3 )O3

Pb(Zn1/3Nb 2/3)O3 is a relaxor ferroelectric which can be used in single crystal


form. Figure 8.5 shows the birefringence ∆n versus electric field E relation for a
Pb(Zn1/3Nb 2/3)O3 single crystal in the paraelectric phase.3) The single crystal
sample was made by a flux method using excess PbO. The parabolic curve in the
low field region becomes a straight line in the high field region.
226 Chapter 8

Fig. 8.5 Birefringence vs. electric field response of paraelectric


Pb(Zn1/3Nb 2/3)O3 .

A possible phenomenological analysis of this peculiar phenomenon is based on the


model that the crystal is composed of coexisting ferroelectric and paraelectric
phases.3) Suppose that the volume fraction of the paraelectric phase x(T) is given
by an accumulated Gaussian distribution with respect to temperature, the
birefringence ∆n is estimated by the summation of the linear and quadratic
electrooptic effects:4)

∆n = [1 - x(T)] n 3 (r 33 - r 13 ) E/2 + x(T) n 3 R44 E2/2, (8.3)

where n is the refractive index, and r and R represent the electrooptic Pockels and
Kerr coefficients, respectively. Even if the experimental data can be represented
phenomenologically, the actual situation may not be so simple as this model
predicts as x(T) is also a function of the applied electric field E.

Another more realistic description is found in terms of a microscopic domain


reversal mechanism. Pb(Zn1/3Nb 2/3)O 3 has very small spindle-like domains (5
µm) with ambiguous boundaries arranged perpendicular to the external electric
field. When a field greater than 0.5 kV/mm is applied, the domain walls within a
certain region of the sample moves togeter, such that the micro-domains respond to
the applied field in a cooperative manner (See Fig. 8.6). 5) It is noteworthy that the
stripe period of the dark and bright domains (corresponding to up and down
polarizations) will not be changed by domain reversal, and that each domain area
Electrooptic Devices 227

changes under an AC external field with zero net polarization at zero field. The
relaxor crystal can be electrically poled easily when an electric field is applied
around the transition temperature, and depoled completely without any remanent
polarization. This is the basis of the large "apparent" secondary non-linear effects
such as electrostrictive and electrooptic Kerr phenomena, which occur without any
hysteresis.

E // <111>

Fig. 8.6 Domain reversal mechanism in Pb(Zn 1/3Nb 2/3)O 3.


228 Chapter 8

(3) Pb(Mg 1/3 Nb2/3 )O3 -PbTiO3

The development of new ceramic electrooptic materials with higher fracture


toughness and larger electrooptic coefficients suitable for image display
applications is necessary. The following conditions should be considered:

1) ceramic transparency requires almost zero birefringence in the zero-field


state (that is, a pseudo-cubic structure) to suppress light scattering,
2) large fracture toughness may be obtained in a sufficiently dense structure
(that is, ion vacancies are not suitable),
3) a large electrooptic effect is manifested by relaxor ferroelectrics.

The Pb(Mg1/3Nb 2/3)O3 -PbTiO 3 system, which is known as a superior electro-


strictive (secondary effect) material with very high fracture toughness (KIC = 1.7
MNm-3/2 ) is a good candidate for electrooptic applications.6) Samples of the (1 - x)
Pb (Mg1/3Nb 2/3)O3 - x PbTiO3 system were prepared by hot-press sintering of
oxide mixtures. The Curie temperature increases gradually with PbTiO 3 content,
passing room temperature around x = 0.12, and the crystal structure is pseudo-cubic
in the region below x = 0.4. Figure 8.7 shows the composition x dependence of
optical transmittance (λ = 633 nm) of a 0.5 mm thick sample from the (1 - x)
Pb(Mg1/3Nb 2/3)O3 - x PbTiO3 system. The transmittance is reduced drastically
above x = 0.14, probably due to scattering caused by the spontaneous birefringence.
The best transmittance 49% is still smaller than the 62% observed for PLZT. This
suggests that a more sophisticated powder preparation technique will be required for
fabricating adequately transparent PMN-PT ceramics.

Fig. 8.7 Transmittance of a 0.5 mm thick sample of (1 - x) Pb(Mg1/3Nb 2/3)O 3- x


PbTiO3 (λ = 633 nm).
Electrooptic Devices 229

The refractive index n (λ = 633 nm) is plotted as a function of composition x in Fig.


8.8, and shows a small maximum around x = 0.12. The values are slightly larger
than the n = 2.49 of PLZT 10/65/35. The most interesting data come from
electrooptic measurements. Figures 8.9(a) and 8.9(b) show the electrooptic R
coefficient and its corresponding hysteresis for λ = 633 nm, respectively, plotted as
a function of composition x. The maximum electrooptic R coefficient of 22 x 10-16
m2 V-2 for x = 0.12 is more than twice that of PLZT 9/65/35 (9.1 x 10-16 m2 V-2 ).
The hysteresis, defined as an equivalent coercive electric field obtained from the
experimental ∆n curve, increases drastically above x = 0.16 and, hence, samples in
this region cannot be used practically.

Fig. 8.8 Refractive index as a function of composition x for (1 - x) Pb(Mg1/3


Nb 2/3)O 3 - xPbTiO3.

Fig. 8.9 Changes in the electrooptic coefficient R (a) and the corresponding
hysteresis (b) in (1 - x)Pb(Mg 1/3Nb 2/3)O 3 - xPbTiO3.
230 Chapter 8

The data indicate that the 0.88Pb(Mg1/3Nb 2/3)O 3-0.12PbTiO3 has the potential to
be a better electrooptic ceramic than PLZT with high mechanical toughness. Higher
optical transmittance must be achieved, however, by optimizing the fabrication
process.

8.3 BULK ELECTROOPTIC DEVICES


(1) Ferpic

One of the earliest applications is Ferpic (Ferroelectric Picture Memory Device).


Figure 8.10 shows the principle of the Ferpic.7) Initally, a PLZT 7/65/35 ceramic
plate is uniformly DC-poled laterally [see Fig. 8.10(a)]. Then, storage is achieved
by switching domains at points corresponding to the image's high-intensity regions.
To switch domains, a high-contrast transparency is placed in front of the Ferpic and
illuminated [Fig. 8.10 (b)], creating low-impedance regions in the photoconductive
film. The writing voltage supply will then cause switching in these regions only.

Viewing/reading the memorized image is accomplished by passing polarized light


through the Ferpic and an analyzer as shown in Fig. 8.10(c). When the polarizer
and analyzer are parallel, the regions with remnant polarization normal to the plate
produce a bright image, and the other regions produce a dark image.

(2) Eye Protection Application

Sandia National Laboratories designed PLZT goggles for the U.S. Air Force to
provide thermal and flashblindness protection for aircraft personnel.8) The goggle is
basically a transverse-mode shutter using an interdigital surface electrode
configuration similar to that shown in Fig. 8.11.

(3) Stereo TV Application

PLZT eye glasses for stereo TV (see Fig. 8.11) have been fabricated using the light
shutter principle. 9) The lenses consist of a pair of optically isotropic PLZT
(9/65/35) discs sandwiched between two crossed polarizers. When zero voltage is
present between the electrodes, light will not be transmitted. The transmitted light
intensity increases with increasing applied voltage, and reaches a maximum when a
phase difference (retardation) of 180o is induced in the PLZT disc (at the half-wave
voltage).

Stereo TV images of an object are taken by two video cameras corresponding to the
two eyes and the signal from each camera is mixed alternately to make a frame for
the right and left eyes. When viewing, the right and left PLZT shutters are triggered
synchronously to each image frame, resulting in a stereo image.
Electrooptic Devices 231

Fig. 8.10 Principle of Ferpic: (a) initial DC poling, (b) writing process using a
photoconductive film, (c) reading process using a pair of parallel polarizers.
232 Chapter 8

TV cameras
left right

left image right image

PLZT glasses

Fig. 8.11 A stereo TV system using a pair of PLZT glasses.

(4) Two-Dimensional Displays

The current requirements for high definition TV are stringent, and several systems
have been proposed. One of the promising devices is a projection type TV utilizing
one-dimensional10) or two-dimensional PLZT displays.11) The operating principle
for a projection TV utilizing two-dimensional PLZT displays is introduced in this
section. The development of a simple mass-production process and the design of
electrode configurations with a narrow gap are the key factors in the production of
the PLZT displays. A design shown in Fig. 8.12 produces a very bright image with
small crosstalk-related problems and is easy to manufacture.

Fabrication Process of the 2-D Display

The fabrication process for the two-dimensional PLZT light valve array is outlined
in Fig. 8.13. 11) Coprecipitated PLZT 9/65/35 powders were mixed with organic
solvent and binder and formed into a green sheet. Platinum internal electrodes were
printed on the green sheets. The electroded sheets were then laminated, with the
electrodes alternating by 90o between sheets, under a pressure of 3000 psi. The
laminated body was sintered in an oxygen-controlled atmosphere, and the bulk was
cut and polished. Finally the external electrodes were applied for vertical and
horizontal addressing for individual pixels on the display.
Electrooptic Devices 233

Fig. 8.12 A two-dimensional PLZT optical display: (a) a matrix segment and (b)
detail of an activated portion of the display.

Figure 8.14(a) shows the electrode configuration of a (10x10) matrix light valve.
The shaded portion of the device in the figure represents one image unit (pixel).
The separated internal electrodes are connected by external electrodes printed on the
surface of the device. The continuous (plate-through) electrodes are embedded 100
µm below the optical surface to avoid shorting with the surface electrodes
connecting the separated internal electrodes. Figure 8.14(b) shows a picture of an
actual display. Note that the layer thickness is about 0.35 mm.

Characteristics of the light valve array

The optical transmittance of the PLZT device fabricated by the tape casting
technique was 62% at λ = 633 nm, which is comparable with 63% transmittance for
the ideal bulk sample prepared by hot-pressing. The brightness for red, green and
blue light was measured as a function of applied voltage (Fig. 8.15), where the
electrode gap was 0.45 mm. 11) The contrast ratio, defined as the ratio of the
brightness on a screen with the application of the half-wave voltage to the
brightness with zero volt applied (220 cd/m2/2.8 cd/m2 ), of about 80, is superior to
the values for conventional cathode ray tubes (CRT) or liquid crystal displays
(LCD). The response time (both rising and falling) of a single pixel on the display
is less than 10 µsec, which is rapid enough to drive this shutter array at a raster
frequency comparable to the conventional CRT.
234 Chapter 8

Fig. 8.13 Fabrication process for the two-dimensional PLZT optical display.

Construction of the Image Projector

The driving circuit for the display is shown schematically in Fig. 8.16(a). When the
terminals of the device are addressed as shown in Fig. 8.16(b), the image appearing
in Fig. 8.16(c) (letter "F") is generated on the screen.11)
Electrooptic Devices 235

Fig. 8.14 (a) Schematic electrode configuration of a (10x10) matrix PLZT light
valve. (b) Top view photograph of a PLZT light valve array with external
electrodes.

Fig. 8.15 Brightness on a screen vs. applied voltage for red, green or blue light.
Note that the half-wave voltage differs for these three lights.
236 Chapter 8

Fig. 8.16 (a) Driving circuit for the two-dimensional display. (b) The driving
signal waveforms of the driving signal. (c) An image of "F" on a screen illuminated
through the PLZT projector.
Electrooptic Devices 237

Fig. 8.17 Crosstalk test system. The light through a slit focused on the screen is
measured.

Fig. 8.18 Crosstalk patterns for three different input combinations: (a) vertical
type, (b) oblique type and (c) complex type.
238 Chapter 8

Crosstalk was monitored on the 2-D display using the setup shown in Fig. 8.17 with
monochromatic light.6) The test was made by keeping one vertical terminal
(separated electrode) on (i.e., Ground) and applying high voltage to multiple
horizontal terminals (continuous plate-through electrodes) simultaneously. There
are three different crosstalk patterns: vertical, horizontal and oblique types; that is,
light leakage observed at vertically, horizontally and obliquely adjacent pixels. The
results are shown in Fig. 8.18(a)-(c) for three different input combinations, where
the top and bottom of figures in a pixel indicate the light intensity in µW on the
screen for the ON and OFF state, respectively. The leakage light intensity
associated with the vertical and horizontal crosstalk is 20 - 30% and 10 - 20% of the
main-peak intensity, respectively, which does not affect the image contrast
significantly. On the other hand, oblique type crosstalk causes non-negligible
leakage, up to 50% depending on the applied voltage and the number of continuous
electrodes addressed (horizontal address) (called combination type crosstalk).
Modification of the internal electrode configurations is necessary to eliminate the
crosstalk problem completely.

Example Problem 8.2_________________________________________________

In Fig. 8.15, the first maximum in the light intensity is obtained at different voltages
for red, green and blue light; 160 V for red, 150 V for green and 130 V for blue.
(1) Explain the reason physically.
(2) Supposing that the refractive index n (= 2.49) and the electrooptic coefficient
(R 11 - R12) (3.6 x 10-16 [m2/ V2]) does not change significantly for each light,
calculate the wavelength of these three lights.

Hint

The half wave voltage is calculated from

Γy = (p/λ) n 0 3 E3 2 (R 11 - R12 ) L
=π. (P8.2.1)

Solution

(1) Since the half wave voltage is provided by Eq. (P8.2.1), according to the
illumination light wavelength, the required voltage differs: for shorter
wavelengths, a smaller electric field is required.

λ = n 0 3 E32 (R 11 - R12) L . (P8.2.2)

(2) Taking into account the electrode gap of 0.45 mm, E3 = 3.55, 3.33 and 2.89 x
10 5 [V/m] for R, G and B, respectively, and a pathlength L given by (1.0 - 0.1)
mm (note that the surface depth 0.1 mm is an inactive layer):
Electrooptic Devices 239

λ = 2.493 x (3.55x105 )2 (3.6 x 10-16 ) (0.9 x 10-3)


= 630 [nm] (for red),

λ = 555 [nm] (for green),

λ = 418 [nm] (for blue). (P8.2.3)


___________________________________________________________________

8.4 WAVEGUIDE MODULATORS

Light waveguides can be fabricated by depositing a high-refractive index layer on a


substrate. The principle of the waveguide is shown schematically in Fig. 8.19.12)
Like an optical fiber, the light tends to bend toward high refractive-index side, so
that the light should be confined in the narrow high refractive-index layer fabricated
on the crystal. Nb-diffused LiNbO3 single crystals are commonly used. Figures
8.20(a) and 8.20(b) are typical planar and ridge type electrooptic waveguides.13)
The fabrication of a planar type is easy, but the nonuniform distribution of the
applied electric field is a problem. On the other hand, as you can imagine, the ridge
type requires sophisticated manufacturing technology, but the device function is
close to the ideal. The transmitted light intensity is easily modulated by applying a
relatively low voltage. Phase modulation by 1 radian can be achieved by applying a
voltage of 0.3 V with power consumption of several µW/MHz.

Fig. 8.19 Diagrams of (a) slab and (b) graded-index waveguides. The wave-
functions for the TE0 and TE1 modes are shown in the refractive-index profiles.12)
240 Chapter 8

Fig. 8.20 Electrooptic waveguides: (a) planar-type and (b) ridge-type.12)

CHAPTER ESSENTIALS_________________________________
1. Relaxor ferroelectrics are widely applicable for electrooptic light valve/display
applications. The superior characteristics of these materials are attributed
primarily to the easy poling of the ferroelectric micro-domains.

2. A new electrooptic ceramic 0.88Pb(Mg 1/3Nb 2/3)O 3 -0.12PbTiO3 with high


mechanical toughness is one of the more promising new materials for long-
lifetime display applications.

3. A new type of PLZT two-dimensional light valve, fabricated by a tape casting


technique, is one excellent example of a design well-suited to mass-production
at a low manufacturing cost.

4. Light waveguides can be fabricated by depositing a high refractive index layer


on a substrate such as LiNbO3 .
___________________________________________________________________
Electrooptic Devices 241

CHAPTER PROBLEMS

8.1 Let us consider a PLZT thin film (1 µm in thickness) deposited on a glass


plate with the following two electrode configurations: (a) surface electrode
for lateral electric field and (b) surface electrode for normal electric field.

Light direction
(a)

PLZT film

Light direction
(b)

(1) Discuss the merits and demerits of the above two electrode
configurations.

(2) Suppose that the electrode in part (b) of the figure above is made of a
transparent material such as SnO2. Do you think the device will work for
light transmitted normal to the film?

Hint

Consider the birefringence and the shape of the optical indicatrix induced
by the electric field.

8.2 Consider Kerr electrooptic effect for a crystal with m3m symmetry.

(1) Derive a secondary electrooptic coefficient matrix for this symmetry.

(2) Discuss the change in the optical ni dicatrix shape (refractive index
ellipsoid), when an electric field is applied along the z axis.

(3) Calculate the retardation, when the light is transmitted perpendicular to


the electric field, that is, along the y axis. The pathlength is L.
242 Chapter 8

Hint

The electrooptic coefficient matrix is given as

R 11 R 12 R 12 0 0 0
R 12 R 11 R 12 0 0 0
R 12 R 12 R 11 0 0 0
0 0 0 R 44 0 0
0 0 0 0 R 44 0
0 0 0 0 0 R 44

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Appl. (Kyoto) p.155 (1977).
4) J. Kuwata, K. Uchino and S. Nomura: Ferroelectrics 22, 863 (1979).
5) R. Ujiie and K. Uchino: Proc. IEEE Ultrasonic Sympl (Hawaii) p.725 (1990).
6) K. Uchino: Ceramics International 21, 309 (1995).
7) L. M. Levinson edit.: Electronic Ceramics, Marcel Dekker (New York), Chap.7,
p.371 (1988).
8) J. T. Cutchen: Proc. 49th Annual Sci. Mtg. Aerospace Medical Assoc., New
Orleans, May (1978).
9) A. Kumada, K. Kitta, K. Kato and T. Komata: Proc. Ferroelectric Mater. & Appl.,
2, p.205 (1977).
10) K. Murano: Ceramic Transactions 14 Electro-Optics and Nonlinear Optic
Materials, p.283 (1990).
11) K. Uchino, K. Tokiwa, J. Giniewicz, Y. Murai and K. Ohmura: Ceramic
Transactions 14 Electro-Optics and Nonlinear Optic Materials, p.297 (1990).
12) M. E. Lines and A. M. Glass: Principles and Applications of Ferroelectrics and
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