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ULTRASONICS,
ON
AND
SONICS
481
Rod-Polymer Composites
IEEE,
IEEE,
AND
Abstmcr-Theobjective
of thepresentworkwastogainadeeper
mensions of the transducer are muchsmallerthanthe
understanding of the behaviorof lead zirconate titanate (PZT) polymer acoustic wavelength [ l]-[8]. Until now there have been no
composites for applications such as ultrasonic medical diagnosis in the
studies investigating the usefulness of these composites at
megahertzfrequencyrange.Thesecompositeswereoriginally
develhigher
frequencies (1-10 MHz) for medical diagnostic and
oped for low-frequency hydrophone applications. The PZT rod-polynondestructive
testing applications. At these frequencies,
mer composites have been prepared with
five to 30 volume percent PZT
using 0.28 mm and 0.45 mm rods. In a disc of PZT rod-polymer com- the acoustic wavelength is comparable to the scale of the
posite material, there are three principal types
of resonance: the planar composite microstructure. Theacoustic impedance, bandmode, the thickness mode, and various lateral modes caused
by the regwidth, and radiation patterns of the composite transducer
ular periodicityof the PZT rod in the composite. These resonance modes
have been studied with the following techniques:
1) electrical impedance can be controlled in a manner so sophisticated that it is
measurement as a functionof frequency and 2) laser probe dilatometry impossible in single phase materials. The results of a sysof the dynamic displacementas a function of frequency and position in tematicinvestigation
of thecompositematerialsmade
the composite lattice. The observed resonance behavior is found to be frompiezoelectric lead zirconate titanate (PZT) ceramics
a result of lateral interactions in the composite through the epoxy meand piezoelectrically inactive polymer are reported here.
dium. The effect of temperature on the electromechanical properties
of electromeThisstudyfocusesontheunderstanding
of the composite has also been investigated. Implications
of these results
chanical
properties
of
the
composite
materials
in resonant
for optimizing the design of ultrasonic transducers are discussed.
configurations. The knowledge of the high-frequency dynamic behaviorof the composite was then used to evaluate
thecompositematerialsforultrasonictransducerappliI. INTRODUCTION
cations with an emphasis on medical diagnostic applicaHE DESIGN and fabrication of composite materials tions. These results are discussedin an accompanying paoptimized for a special application has been the sub- per (Part 11).
In Section I1 the requirements of a piezoelectric transject of extensive research recently. The applications range
ducer
for ultrasonic imaging applications and the
limitafrommechanicalstructures to electronic devices.In detions
of
the
existing
single
phase
transducer
materials
are
signing composite materials, primary importance is given
described.
In
Section
1
1
1
a
brief
review
of
the
earlier
works
to the proper choice of component phases and the way in
on piezoelectric ceramic-polymer composites of relevance
which they are interconnected to maximize a predefined
tothepresent
work isgiven.Advantages
of theuse of
figure of merit for the application envisaged.An important
for
ultrasonic
applications
are
pointed
out. The
composites
class of these new materials is the family of piezoelectric
criteria
used
to
select
an
appropriate
composite
structure
ceramic-polymer composite transducers. To date, most of
the work on piezoelectric ceramic-polymer composite ma- for a detailed investigation for high frequency transducer
terials has been focused on hydrophone applications in theapplications are also described. Bulk mechanical properlow-frequency(lessthan 40 KHz) range,where the di- ties of the polymer phase that strongly influence ultrasonic
properties of the composite are summarizedin Section IV.
The characterization of all the different resonance modes
ManuscriptreceivedNovember 26, 1984. This work was supported in
in the composite are discussed in Section V. Laser probe
part by North American Phillips Laboratories.
T. R. Gururaja, L. E. Cross, and R. E. Newnham are with the Materials measurements are presented in Section VI. The effect of
Research Laboratory, The Pennsylvania State University, University Park,
temperature on the resonance modesin the composite are
PA 16802, USA.
VII. Finally, the implication of the
B. A. Auld and Y.J . Wang, are with the Edward L. Ginzton Laboratory, dealt with in Section
Stanford University, Stanford, CA 94305, USA.
resultson thehigh-frequencyvibrationbehavior
of the
W. A. Schulze was with the Materials Research Laboratory, The Penncomposites
in
air
for
the
ultrasonic
imaging
applications
sylvania State University. He is now with the New York State College of
are summarized in Section VIII.
Ceramics, Alfred University, Alfred, NY 14802, USA.
482
TRANSACTIONS
IEEE
111. COMPOSITEPIEZOELECTRICTRANSDUCERS
value, a matching layer mustbepreparedsynthetically,
which isnot always easy. However,in practice,such maPZTceramic, which is commonlyusedasapiezoelectransducer material, suffersfromseveraldisadvanterial is prepared by mixing suitablemetallicpowdersuchtric
as aluminum with some epoxy resin [lo], 1131, [ 141. The tages when used as a hydrostatic pressure sensor. The hycomposite matching layer configurations have relatively drostatic piezoelectric coefficient dh ( =d33 + 2d3,)of PZT
large attenuation coefficientandadd
to further loss of is low due to opposite signs of piezoelectric strain coeffiacoustic
cients d33and magnitudes
d 3 though
,the
,even
of both d33
energy.
11. PIEZOELECTRIC
TRANSDUCER
MATERIAL
PARAMETERS
483
TABLE I
DIELECTRIC
AND PIEZOELECTRICPROPERTIES
OF
PZT-POLYMER
COMPOSITES
Density
(gm/cc)
Dielectric
Constant
K
7.6
1800
2.5
40
Coral replamine-PZT
composite
PZT-Spurns epoxy (BURPS)
PZT-silicone rubber (BURPS)
3.3
50
4.5
4.0
620
450
140
20
45
36
110
180
5040
,2200
8100
1-3
1.4
1.4
54
40
56
56
27
20
1536
1100
1-3-0
1.3
78
60
41
2460
0.9
41
210
73
14600
PbTi0,-chloroprene rubber
Bi,03 modified PbTi03chloroprenerubber
40
100
35
3500
40
28
10
280
3-1
2.6
650
30
170
5100
3-2
2.5
375
60
200
12000
Description
of Composite
3-3
0-3
g,
VmN-')
dh @CP.-')
dhgh( 1 0 - % * ~ - ' )
Reference
100
484
4, JULY 1985
TABLE I1
PHYSICAL, DIELECTRIC,
A N D PIEZOELECTRIC PROPERTIES
OF PZT ROD-POLYMER
COMPOSITES
Rod
Diameter
(mm)
Volume percent
PZT
~~
5
10
0.45
10
0.28
1.78
1.26
0.90
1.41
1.64
320 2.29
0.45
0.28
0.73
0.78
0.55
3 .OS
1.62
339 2.36
0.45
0.45
20
Single Phase
PZT
Density
p(gm/cc)
Dielectric
Permittivity K
d~ Coefficient
( pUN)
20
30
Periodicity
d (mm)
400
7.6
375
19
155
I09
I94
238
3 80
94
217
183
1400
ated in a half-wavelengththicknessmodeformaximum
sensitivity. Thus, the major requirement of a composite
was to have a well defined thickness resonance with a reasonably good piezoelectric coupling coefficient and a low
Q. Pulse-echoamplitudeandbandwidthofair-backed
compositetransducersoperating with water load in the
low megahertz frequency range determined by the toneburst pulse-echo method [22] were used as additional parameters.
Amongallthedifferentcomposites,onlythose
with
PZT rods embedded in Spurrs epoxy' matrix with regular
periodicity (1-3 connectivity) appeared to be very promFig. 1. Typical 1-3 composites with PZT rods embedded in Spurrs epoxy.
isingfor the ultrasonic transducer application[21]. The
thicknesscouplingcoefficientfor
thesecomposites was
ers [3]. In brief, PZT-501A2 rods were extruded using an
determined to be about 60-70 percent. This value comorganic binder and then firedat 1285C for one half hour.
pares favorably with the thickness coupling coefficient of
Fired rods were aligned using an array
of appropriately
49 percent for the PZT-5 disc which is used
in commercial
spaced holes drilled in a pair of brass discs boltedparallel
transducers. Mechanical Q of the composites was low (3to eachother. The array of PZT rods wasthencastin
10) compared to that of PZT-5 (80). The pulse-echo amSpurrs epoxy matrix.The resultingcomposite was cut
plitude of these composite transducers was large (from 2perpendicular to the length of the rod and lapped to the
3 V to 10 V input signal) and comparable to those of comrequiredthickness.Thecomposite
wasthenelectroded
merciallyavailable transducers.The 1-3 composites had
with silver paint on the major surfaces and poled convenadditional advantages. There aremany variables including
tionally by applying an electric field of 20 kV/cm for five
PZT rod diameter andvolumepercent
of the PZT and
minutes in a heated oil bath at80C. Different composites
polymer phases, which can be vaned relatively easily to
werepreparedwithapproximatelyfive,
ten, 20, and 30
optimizetheproperties
for particular application. The
volume percent PZT using 0.45 mm rods and with ten and
continuous poling technique [23] can be used to polarize
20 volume percent PZT using 0.28 mm rods.
Table I1 gives
long PZT rods, which can then be arranged in a polymer
the periodicity (distance between the centersof neighbormatrix in such a way to obtain a desired radiation pattern.
ing PZT rods) of PZT rods in each of these composites.
Since the composite structure resembles a transducer arof
ray, the knowledge of the high-frequency dynamic behav- The composite samples were shaped as circular discs
diameter 19 mm and varying thickness from 0.5 mm to 5
ior of these composites might be helpful in resolving some
mm. A picture of typical compositesamplesisgivenin
of the problems encountered in array applications, such as
Fig.1.
minimizing the acoustic cross talk between the adjacent
Results on the average properties including density, pielements.Because of theseadvantages, 1-3 composites
ezoelectric d33 coefficient,anddielectricpermittivity
of
were chosen for an extensive investigation aimed at high
PZT rod-polymer composites have been reported earlier
frequency transducer applications.
by Klicker et al. [3]. Data for the composite samples used
A detailed procedure for fabricatingcomposites with
1-3 connectivity has been reportedby Klicker and co-work- in this work are listed in Table I1 along with the properties
of single phase PZT-5O1A for comparison.
'Trademark of Polysciences, Warrington, PA.
485
_--.
IV. BULKMECHANICALPROPERTIES
OF
SPURRSEPOXY
Radial Mode
in
Spurrs epoxy is the piezoelectricallyinactivephase
thecompositematerialconsideredhere.
However, its
function in thecompositetransducer
is quitecritical.
When the composite is used as an ultrasonic transmitter,
the epoxy has to effectively couple the ultrasonic energy
fromahigh-acoustic-impedance PZT to a low-acousticimpedance load. Similarly, in the receiving mode, the ul(b)
trasonic energy incident on the composite shouldbe transferred effectively to the piezoelectrically active PZT. The Fig. 2. Resonance modes in a disc-shapedpiezoelectricmaterial.(a) Radial mode. (b) Thickness mode.
importantparameters of thepolymerthatinfluencethe
performance of the composite as an ultrasonic transducer
are its acoustic impedance, longitudinal and shear wave A . Planar-ModeResonance
velocities,and attenuation coefficients and their depenThe planar mode (alsocalledradial)vibrationinthin
dence on frequency. These properties of the polymer dedisc, as illustrated in Figure 2(a), involves simultaneous
termine the interaction among the neighboring PZT rods
mechanical motion in the 1 and 2 directions driven by the
andhencethehigh-frequencydynamicbehavior
of the
(poling
direction).
electric field in the 3 direction
composite.Measurementtechniques
used to determine
Since the diameter was the largest dimension (19 mm) in
these parameters in Spurrs epoxy are described elsewhere
all the composite samples, the planar mode was thelowest
[24]. Only the results which are useful for analysis of the
frequency resonance mode.
vibration behavior of the composites are presented here.
TheIRE(nowIEEE)standardon
piezoelectricmeaThe longitudinal andtransverse
wave velocities in
surements
[26]
was
used
to
determine
the
electromechanSpurrs epoxy were determined to be 2060 m/s and 1150
ical
coefficients
and
elastic
constants.
The
most important
m/s, respectively. The acoustic impedance of the Spurrs
parameters
for
calculating
these
constants
are the series
epoxy was calculated to be 2.27 X lo6 kg/m2-s. The atand parallel resonance frequenciesf, and&, the geometric
tenuation of the transversewave in Spurrs epoxywas measured to be 6 dB/cm at 0.5 MHz. The attenuation coeffi- capacitance C,, and the impedance minimum lZ,l at rescient wasfound
to increase with thesquare
of the onance. A spectrumanalyzer(HP 3585A), which provides a circuitsimilar to the transmissionnetworkrecfrequency. The glass transition temperature Tg is another
ommended by the IRE standard, was used in measuring
characteristic parameter for polymeric material. The
glass
frequencies fm and f, corresponding to minimumand maxtransition temperature is defined as the temperaturebelow
imumimpedance. In thepresence of highmechanical
which the material behaves like a glass and above which
losses, fm andf, are quitedifferent fromfs and&. TheIRE
thematerial is rubberlike andsoft [25]. In the present
Standard recommends the following approximation to calwork Tg and its dependence on frequency was determined
culate Af = fp - fs from the measured value off, and f,
by measuring the dielectric loss tangent of Spurrs epoxy
as a function of temperature and frequency. At the glass L261
transition temperature,the loss tangentgoesthrougha
peakandcanbeeasilyidentified.ForSpurrsepoxy,
TR
was found tobe a functionof frequency varying from 70C
at 1 0 0 Hz to 121C at 1 MHz with a shift of 12-15C per
where the figure of merit M is given by
decade of frequency.
P
V. RESONANCEMODES
1
2rfJ1Co
M =
2nfm(Co + CI)lzml.
(2)
l + a
IEEE TRANSACTIONS ON SONICS AND ULTRASONICS. VOL. SU-32. NO. 4. JULY 1985
486
TABLE 111
ELECTROMECHANICAL
PROPERTIES OF COMPOSITES FROM THE RADIALMODERESONANCE
Thickness
5
(0.45 mm)
l0
(0.45 mm)
20
(0.45 mm)
30
(0.45 mm)
10
(0.28 mm)
20
(0.28 mm)
Thin
Thick
Thin
Thick
Thin
Thick
Thin
Thick
Thin
Thick
Thin
Thick
k,
40
17.0
21.7
36
16.6
1.1
42
1.5 to 2 . 02 3 . 0
1.2
23
21.0
1.5 to 2.3
26.5
34
1.1
20.0
3626.72.0
1.1
18.8
23.11.5
1.1
22.0
25.5
1.7
c*
N(Hzm)
(Frequency
Constants)
Longitudinal
Velocity
(mis)
1483
32
1064
1120
1011
l080
955
1043
950
36
35
32
35
1032
1097
970
1057
0.97
- 1.4
34
1561
1409
1506
l33 1
1454
1324
1458
1439
1529
1352
1474
1046
fraction of PZT. Thick composites have a higher kp comparedto thincomposites of thesame volume fraction.
Lower values of kp in thin samples indicate that the mePZT
chanicalenergy is not efficiently coupledfromthe
rods tothe polymer and from the polymer back
to the PZT
rods. Thecouplingbecomesmore
efficientforthicker
samplesindicating a greater homogeneity. A similarexplanation can be given for the difference in the frequency
constant between the thick and thin samples.
In the last column of Table 111, the longitudinal velocity
C, perpendiculartothelength
of therodislisted.
The
value of C,was calculated using the relation [27]
fs = 2.05
[(E,lp(l
27ra
The calculated values of kp and Q from (3) and ( 5 ) for
several composites are summarized in Table 111. The frequency constant Np for the planar mode (product of resonancefrequencyandthediameter)isalsolisted
in the
table. The data are divided into two groups depending on
the thickness of the sample. The first group investigated
of about 0.6
consisted of thinsampleswithathickness
mm.Thesecondgroup
was comprised of allsamples
thicker than 3 mm and was classifiedas thick samples. The
properties remained virtually constant in the two extreme
limits. The data listed in the table are an average of the
measurements of at least five samples.
As it emerges from Table 111, the figure of merit M for
the radial-mode resonance of all the composites was between one and two. As mentioned before, (3) and ( 5 ) used
for calculating kp and Q are not fully valid for values of
M < 3. Subsequently, the valuesof kpand Q listed in Table
111 are far from being exact. However, since the value of
M is approximately the same for all the samples, the uncertainty in assessing k,,, and Q is of the sameorder. Hence
the results can be used for a relative comparison of samples having different volume fraction PZT.
Table I11 indicates that the planar coupling
coefficient k,,
of the composites increases with increase in the volume
- C?)]*
_1 -- _U1 + -2
Et
E,
E2
(7)
l300
I
IO
20
30
l
40
50
Fig. 3. Longitudinal velocity perpendicular to the PZT rod axis as a function of volume percent PZT In composites.
487
IEEE TRANSACTIONS ON SONICS AND ULTRASONICS. VOL. SU-32, NO. 4, JULY 1985
488
TABLE IV
COMPARISON
OF IRE STANDARD METHOD
A N D VECTOR IMPEDANCE METHOD
FOR CALCULATING
ELECTROMECHANICAL COUPLING COEFFICIENTS'
Standard
Sample
Thickness
in mm
200
20 1
202
203
204
205
0.66
2.54
3.05
3.95
4.60
5.15
fm
IRE
- f,
Af= fp
-L
(KHz)
(KHz)
2.320
1.820
1.998
2.225
2.386
2.842
1.0
1.7
1.041
1.168
1.364
1.585
1.760
2.172
1.9
2.0
2.2
2.4
Vector Impedance
Method
Method
Kp (%)
24
22.6
39
22.8 0.929
37
24.7
26.41.48035
35
21.8
30.81.79230
fp -fs
kp (%)
0.350 72 12.9
48 20.3
1.184 43 22.9
25.6
27.1
1.711
27.8
39
37
37
489
TABLE V
THICKNESS-MODE RESONANCE
I N COMPOSITES
Longitudinal
Frequency
Velocity
Constant
Nf (Hz m)
(mis)
Thickness
(mm)
Figure of
Merit M
k,
percent
5
(0.45)
0.6
4 to 6
2.4
57.1
27.5
31
1834
1327
3668
2654
10
(0.45)
0.6
3.6
4-6
4-6
68.0
40.0
7
23
1820
1492
3640
2984
20
(0.45)
0.6
3 to 5
5-7
5-7
68.9
9
1603 18
55.1
1853
3706
3203
2.2
c,
2NP
30
(0.45)
2.4
12
61.1
26
1687
3374
10
(0.28)
0.6
3-5
3.6
62.6
40.6
4
22
1956
1403
2912
2806
20
0.6
2.9 to 3.4
5-7
72.0
5-7
50.0
8
25
1874
1555
3748
3110
1.9
(0.28)
C. Lateral-ModeResonances
In additiontotheradial-andthickness-moderesonancesandtheirovertones,otherresonanceswereobserved in the frequency range 0-2 MHz. The frequencies
of these resonances were independentof sample thickness,
but were related to the lateral periodicityof the PZT rods
in the composite. Absolute value of electrical admittance
was measured on samples as a function
of frequency in the
ambience of air and waterusing a spectrum analyzer (HP
3585A). Here samples of different thickness and volume
2000
0
IO
20
30
40
50
fractionwereexaminedtoidentifythedifferentresoVolume Percent PZT
nances observed in the 0 to 2 MHz frequency range. Three
Fig. 5. Longitudinal velocity along the PZT rod axis as a function of vol- major resonances of interest are designated as fi, AI, and
ume percent PZT in composites.
A2 as categorized in Table VI.
The resonance corresponding to fi was inversely proportional to the thickness of the sample. This resonance
The longitudinal velocity Cl along the length of the rod
was heavily damped when the resonator was immersed in
canbetheoretically estimated by calculatingtheelastic
water. Such behavior suggests that resonance
at fi is the
modulus EI of the composite parallel to the PZT rods. At
longitudinal thickness vibration. The longitudinal velocity
wavelength is much
frequencieswherethetransverse
of sound, calculated usingtheformula Cl = 2tf, agrees
larger than the separation distance between the rods, the
very well withthetheoreticallyestimatedvalueforthe
Voigt constant strain model [l41 can be applied. The comcomposites of different volume fractions, as discussed in
posite modulus using the Voigt average is written as
detail in the previous section.
The resonances at&, and&? were
very similar in nature.
El = u , E ~+ u ? E ~
(11)
For a certain volume fraction, these resonances
always ocwhere El and E2 arethemoduli,and
u I and u2 a rethe curred at specified frequencies regardless of the thickness
volume fractions of the two phases (PZT and epoxy). For of the sample. As can be seen in Table VI, increase in the
PZT rods witha diameter that is small compared to length,volume fraction results in closer spacings of rods (reducA2 move to
themodulusalongthelength
is given by E = l/$: = tion of the unit cell) and the resonances and
10.5 x 10" N/m2(the Young's modulus of the rod at con- higher frequencies.
The behavior of the composites could be explained by
stant electric displacement). The longitudinal velocity Cl
simpleaveragingschemessuchastheconstantstrain
was calculated from the relation Cl = (El/p)"2.
The experimentally determined longitudinal velocity Cl, model and the constant stress model forwavelengths large
expressed as twice the frequency constant @, is given in or small compared to the lattice periodicity (Section V-A
the last column of Table V. This velocity is compared with and V-B). In the vicinity of the resonances of A, and A2,
the calculated values in Fig. 5. The excellent agreement the wavelength of the transverse shearwave is comparable
to the unit cell dimensions of the array and the analysis is
betweentheexperimentalandtheoreticalvaluesfurther
morecomplicated.
A Brillouintheory of elastic wave
supports the equal strain model for calculating the effecin a twodimensionallyperiodiclatticecortivemodulusofthecompositealongtherodaxis.propagation
40001
IEEE TRANSACTIONS ON SONICS AND ULTRASONICS, VOL. SU-32, NO. 4. JULY 1985
490
TABLE V I
R E S O N , ~ NMODES
T
IK COMPOSITE M A T E R I A L S
Resonance Frequency
.
. in
KHz
Percent
Volume
10
20
20
30
30
Rod
Thickness
Periodicity
c, = dfil
(1
= -r
v2
51
52
53
54
0.45
0.45
0.45
0.45
2.59
4.00
4.80
5 .90
604
1.58
1.76
1.76
1.76
437
450
3I2
262
222
483
449
101
I02
103
0.45
0.45
0.45
1.93
3.64
5. 15
I .27
1.27
1.27
604
410
262
804
662
644
1096
1006
2294
2984
2698
102 1
840
72 1
984
903
I
202
203
204
205
0.45
0.45
0.45
0.45
0.45
2.54
3 .OS
3.95
4.60
5.15
0.90
0.90
0.90
0.90
0.90
540
455
348
296
270
894
830
828
886
825
2742
2774
2748
2722
2780
804
747
745
792
742
I
302
0 45
0.45
2.44
5.15
0.73
0.73
569.5
276.5
1125
1188
2778
2848
82 1
867
(a)
(b)
786
691
c, = 2tfi
730
8782330
2496
25 l4
908261 8
954
853
790
769
859
GURURAJA
M.4TERIALS-PART
er al.:
COMPOSITE
PIEZOELECTRIC
49 1
40
predictedtobezero;andthishasbeen
verified experimentally. The velocity C,, of transverse waves, as tabulated in the last two columns of Table VI is lower than the
measured velocity of 1150 m/s (Section V). Thisispossibly due to the mass loading by the PZT rods.
400
IO00
Frequency ( K H z )
I600
f,,
492
4, JULY 1985
e
I
(mm)
-Position
(mm)
-60-
Position
ON THE
VII. EFFECTOF TEMPERATURE
face of the composite is a clear indicationof efficient couRESONANCE
M
ODES
pling of the mechanical energy from PZT to the epoxy.
Sincethe acousticimpedance of the epoxyis relatively
In this section the effect of temperature on the electroclose to that of the human body, an effective coupling of
acoustic energy from the composite transducer to the hu- mechanical properties of the composite is discussed. It is
clear from the preceding sections that the high-frequency
man body is ensured.
GURURAJA et a l . : PIEZOELECTRICCOMPOSITEMATERIALS-PART
493
"
'c
'Or
15
.I
494
IEEETRANSACTIONS
of thickness
thickness 5.15 mm) at different temperatures up to 170C. while to note that above 130"C, the amplitude
Thebehavioris typical of allthick(thickness > 3 mm) mode was increased (Fig. 13(e)-(h)). The secondary lowcomposites.Accordingtotheanalyses
given in thepre- frequencyresonancesclearlyseenat25Cdisappearat
vious section, the three major resonances observed at room
approximately100C.Thisdisappearance
is againastemperature (Fig. 13(a)) were identified as follows.
cribed to the lossy nature of the epoxy around the glass
MHz was identified as ahalf
1) Resonanceat0.262
transition temperature.
wave resonance along the thickness of the composite and
The coupling coefficient k, and Q of the thickness-mode
resonance for sample 130 are plotted as a function of temis denoted byf,.
2) Resonance at 0.644 MHz was identified as the stand- perature in Figs. 14 and 15, respectively. The value of k,
(0.48)determined atroom temperature(25C)did
not
ing wave pattern in the epoxy arising from lateral periodicity of the PZT rods. This resonance is denoted byf,,. changesubstantiallyuptoapproximately110C.
In the
3) Resonance at 1.030 MHz was identified as the third temperature range from 100 to 130"C, k, exhibited a minimum. Above 130"C, after the transverse mode had disovertone of the thickness mode.
Weak secondaryresonances
below thefrequency of appeared, k, increasedsignificantly to about 60 percent.
As shown in Fig. 15, the mechanical Q at 25C was about
thickness-mode resonance were ascribed to the overtones
20. The Q remained constant to approximately 100C and
of the planar-mode resonance of the composite disc.
decreased to a value of five at temperatures above 130C.
The effect of temperature on the above resonance modes
The observed coupling coefficient k, and Q in a thick
(Fig. 13.) is explained by the following. As the temperature
was increased from 25"C, the epoxy is expected to me- sample at room temperature were attributed to the strong
chanically soften at a faster rate than PZT. Therefore, the mechanical interaction among PZT rods through the epoxy
resonancefrequency AI, which is mainly determined by matrix. At temperatures above the glass transition temthe elastic modulus of the polymer, decreased at a faster
perature TK = llO"C), the epoxy is rubber like and soft.
rate than the resonance frequency fi, which is defined by As a result, the mechanical interaction among PZT rods
thecompositemodulus E,. As seen in Fig. 13(b)-(d),at
becomesweaker as also indicated by an increase in the
higher temperaturesf,, gradually approachesf, and finally amplitude of the resonance spectrum (Fig. 13(e)-(h)). In
merges withf, at approximately 110C.In the temperature effect, k, of the composite approach kS3 of afreely susrange 11O-13O0C, the two modes interferewith each other. pended PZT rod (70 percent) and Q decreases because of
At temperatures above 130"C, f r l passesthrough h and the damping provided by the lossy polymer. It may be reeventually disappears ata temperature around 135 "C. This called here thatfor a thin (thickness = 0.6 mm) composite
disappearance can be attributed to the fact that above the sample, k, was 60-70 percent, and Q was 3-10 (Table V).
glass transition temperature the epoxy is less viscous and These values are very closetothosemeasuredforthick
cannot support a standing wave pattern of the transverse composites above the temperature TR.It appears that the
wave (glasstransitiontemperature
of Spurrs epoxy is nature of vibration of a thick composite above TK resemaround 110C at 200 KHz, from Section IV). It is worth- bles that of a thin composite at room temperature.
(d)
(h)
Fig. 13. Temperature-dependenc e o f various resonances in a composite
samples (sample # 103). The x axis isthe frequency 0.1 t f l 1 . l MHz and
the y axis is the relative admit!.ance (50 dB).
495
IEEE TRANSACTIONSON
496
SONICS ANDULTRASONICS.
VOL.S U-32,
IO0
200
0
0
Temperature, C
o Cooling Run
H e m n q Run
ACKNOWLEDGMENT
-7
cc
0.60
50
l00
I50
Temperature, C
coeffi-
REFERENCES
In thin samples, since the coupling among the PZT rods [ I ] R . E. Newnham. D. P. Skinner,and L. E. Cross, Connectivity and
525-536,1978.
perature above TR is unlikely to affect the resonance behavior. This seems to be confirmedby the plot of k, versus I?] -, Flexiblecompositetransducers, Muter. Res. Bull., vol. 13,
GURURAJA
er a ! . :
PIEZOELECTRICCOMPOSITEMATERIALS-PART
foratedPZT-polymercompositesforpiezoelectrlctransducerappli-
[8] H
. Banno,and S. Saito,Piezoelectricanddielectricproperties
of
composites of syntheticrubberandPbTiO?andPZT.
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Phys. Jap., vol. 22, Suppl. 2, pp. 67-69. 1983.
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of piezoelectric ceramic transducers. IEEE Trans. Sonics Ultrason.,
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[l11 J. H. Goll and B. A. Auld, Multilayer impedance-matching schemes
for broadbanding of water loaded piezoelectric transducers and high
Q electricalresonators, IEEE Trans. SonicsUlrrason., vol.SU-22,
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[l21 C. S. Desilets, J. D. Fraser, and G. S . Kino, The design of efficient
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[l31 J. Soquet, P. Defranould, and J. Desbois, Design of low-loss widebandultrasonictransducersfor
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[l91 J. C . McGrath, L . Holt, D. M. Jones, and I. M. Ward, Recent measurementsonimproved thick-film piezoelectricPVDFpolymermaterials of hydrophoneapplications,
Ferroelectrics, vol. 50, pp.
13-20, 1983.
[20] S. Y. Lynn, R. E. Newnham, K. A. Klicker, K. Rlttenmyer, A . Safari,
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[21] T. R. Gururaja, W. A.Schulze. T. R. Shrout.A.Safari, L. Webster,
and L. E. Cross, High-frequency applications of PZT-polymer composite materials, Ferroelecfrics, vol. 39, pp. 1245-1248, 1981.
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[24] T. R.Guraraja, W. A. Schulze.andL.E.Cross.Bulkmechanical
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[26] IRE standards on piezoelectric crystals: Measurements of Piezoelectricceramics, Proc. IRE, vol.49,pp. 1161-1169. 1961.
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497
_-
>
Pennsylvania
State
University
from
1974 to 1983.
Dr. Schulze hasbeenworking
in theareas of
ferroelectric,piezoelectric,andpyroelectricmaterialsandcomposites.thick-filmmaterialsforcircuitryanddielectrics,
ceramic preparation, second harmonic generation, and electrical property
measurements.
g,
Leslie E. Cross (SM79-F84) was born on August 14, 1923, in Leeds, England. He received the
B.Sc.andPh.D.degrees
in physics fromLeeds
University in 1948 and1952,respectively.
Currently, he is Professor of ElectricalEngineeringandAssociateDirector
of the Materials
ResearchLaboratoryatThePennsylvaniaState
University. Prior to joining ThePennsylvania State
University, in 1961, he held positions with Leeds
University as Lecturer (1948-1951) and as a research associate (1954-1961).
Hisresearchinterestsincludeferroelectricmaterialsandferroic
phenomena;dielectric,piezoelectricandpyroelectriccrystals,ceramicsand
composites; electronic ceramics and their applications, electrostriction and
phase transitions.
Dr. Cross is a member of the National Academy of Engineering and a
Fellow of the American Institute of Physics and the American Ceramic Society.
498