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IEEE TRANSACTIONS

ULTRASONICS,
ON
AND
SONICS

481

VOL. SU-32, NO. 4. JULY 1985

Piezoelectric Composite Materials for Ultrasonic

Transducer Applications. Part I: Resonant

Modes of Vibration of PZT

Rod-Polymer Composites

T. R.GURURAJA, WALTER A. SCHULZE, MEMBER,
ROBERT E. NEWNHAM,BERTRAMA.AULD,

IEEE,

LESLIE E. CROSS, FELLOW,
YUZHONG J. WANG

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 from’piezoelectric 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.

T

As the frequency of operation is increased. the frequency bandwidth Of a transducer is in. ity in the frequency range Of '-lo MHz. SU-32.ustic impedance mismatch. Several intrinsic limitations of PVF2 interface determines the quality factor ( Q broadband na. equivalent load varies from four to seven. This concept has proven to creased the use Of an impedancematching layer Of behighlysuccessful in designingcompositematerials quarter wavelength in thickness and characteristic imped.design and fabrication of different types of piezoelectric jng Optimum acoustic matching. The acoustic impedance matching at the low-impedance load. posites were two to three orders higher than that of the and ducer load [l0]. JULY 1985 . which is commonlyusedasapiezoelectransducer material. PIEZOELECTRIC TRANSDUCER MATERIAL PARAMETERS . Major limitations are mensuch as PZTwithhighelectromechanicalcouplingsuffertioned below.5 kg/m2-s. The transducer the thickness ofthe matching layer decreases.compositematerialsforhydrophoneapplications at low cific requirementsofsensitivity. NO. Since no readily availablematerial has its acousticimpedancenearthis 111. As a a large POrtion terials(ceramic or polymer)arefarfrombeingoptimized of the available energy is transmittedinto the backing ma.thecoupling of the acoustic energy at the transducer-load interface is the electrical impedance of PVF2transducers is high and Poor. and hence pVF. tricalenergyappliedto the transducer. single-phase piezoelectric mamatched backing medium [l0].482 TRANSACTIONS IEEE Desilets er al.the Optimum acousticimpedance of the ing layer for a PZT ceramic disc operating into a water sented here in the next section.sampleswithresonancenearthetypicaloperating fieimpedance load such as that Of the human body. In the first method. In addition PVF2 has dielectric a constant of only be given in units Of IO6 kg/m2-s. a result of the aco.even of both d33 energy. ualize structures with dimensions of the order of a milliThe recent development of piezoelectric polymer mameter or less L91. andSouquet et al. Thus.consisting of PZT and piezoelectrically inactive polymer. [ 121 and Go11 [ 151 have further improved of their the bandwidth and the sensitivity disc transducers usingmultiplelayerimpedancematching schemes. the resonanceof the noise ratio.5 MHz and acts as a major Source of absorption of eleca detrimental effect on range resolution. the dielectric loss is found to diminish the signal to ducer bandwidth. Although the Desilets er complete theoretical and experimental analyses for obtain. First of all. which isnot always easy. ~ e n c e f o r t hall acoustic impedances only l o p C/N.bandwidth. and 1121. COMPOSITEPIEZOELECTRICTRANSDUCERS value. Thus.)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 . is a poor ultrasonic transAs mitter. suffersfromseveraldisadvanterial is prepared by mixing suitablemetallicpowdersuchtric as aluminum with some epoxy resin [lo].The d33coefficient of PVF2 is water.Depending On the 'pe. matched to that of the load to minimize reflection losses which are excellent properties for acoustic imaging with a at the interface. two methods are used to increase the trans. The consequence of a high Q in a transducer ceramics. 1131. The dielectric loss tangent in P V F ~is 0. The resonance behavior is thus high Q (narrow is in general more difficultto match than the piezoelectric bandwidth). as discussed in detail by Collerame et al.transducers.the . reasonable piezoelectric coupling. The hycomposite matching layer configurations have relatively drostatic piezoelectric coefficient dh ( =d33 + 2d3.In the second material combining thedesirable properties of differmethod. However. The quency in medicalultrasound.films[191. PVF2 has a low acoustic ical coupling coefficient forhighsensitivityand 2) The impedance. restrain their extensive use in ultraIt is well known that the piezoelectric ceramic materials sonic imaging applications. piezoelectric element is mechanically damped with a well As discussed previously. forcompletenessabriefsummary is preresponse. and wide-bandwidth frequency response.although recentlysomeresearchers have beensuccessful in producing 1-2 mm thick acoustic impedance Of PZT i' around 30 x lo6 whilethetissues have acoustic impedancenearthat of polarized PVF2. ON SONICS AND ULTRASONICS. at KHz whichdecreases at higher frequencies. which makes should also exhibit good axial and lateral resolutionto vis. [ 141.quite involved.mode.terialssuch aspolyvinylidenefluoride(PVF2)hasopened these requirements can be summarized as follows: 1) The up new possibilities for transducers operating with media piezoelectric material should have a high electromechanof low acoustic impedance I161. [l3] havemade piezoelectricphaseused in the composite. 11. [ 171 ture) of the transducer.in practice.such maPZTceramic. it is very difficult to produce from a Severe disadvantage when Operated with a low. [ 181. 4. 1.Inthereceiver In practice. thetransducerfabrication is short acoustic pulses and receive them with high sensitiv. a composite terialresultingin a lower sensitivity. AlThe basic requirements of a piezoelectric transducer for though two layer matching schemes work very well with ultrasonicdiagnostic imagingare an ability to generate readilyavailable materials.the fabrication difficult. a matching layer mustbepreparedsynthetically.25 at a 'low Pulse-rise time and a Prolonged ring down with 2. VOL. The tages when used as a hydrostatic pressure sensor. and Hunt er al. ante to the geometric Of those Of the transThe hydrostaticpiezoelectric coefficients of thesecornNore ["I. high 933 acousticimpedance of thetransducershouldbe well coefficient.andimpulse frequencies (less than 40 KHz) hasbeen in several papers [1]-[8].for ultrasonicimaging applications. In terms Of the parameters.ent phases might be superior.

defined as the manner in which the individual phases areinterconnected. A as 0-0. the voltage coefficient g33 is low because of the high dielectric constant.03 modified PbTi03chloroprenerubber - 40 100 35 3500 - 40 28 10 280 3-1 Perfodted 3-1 composite 2.4 1. coefficient and lower the dielectric permittivity to augment the hydrostatic d and g coefficients. piezoelectric ceramic particles (PZT. and modified lead titanate) 1-10 p in size are loaded in a polymer matrix [g]. The product of dh and g h listed in Table I was used as the figure of merit for the hydrophone applications.-chloroprene rubber Bi.3 50 4. In composite with 0-3 connectivity. a 3-3 composite comprised of PZT and polymer phases continuously self-connected in three dimensions to give two interlocking skeletons in intimate contact with one another [ 1. PZT polymer composites have several advantages over conventional piezoceramic materials for ultrasonic applications. To improve themagnitude of dh and gh. The composites also have a relatively low mechanical Q (3-10) [21]. These properties of thecompositesappear Alwell suited for thebroadbandwidthapplications. 1-1. the human body can be interrogated at lower ultrasonic energy andthe biological effects of ultrasound. there are tenpossible connectivity patterns designated 3-3.3-2.9 41 210 73 14600 PbTi0. Hydrostatic d and g coefficients were measured by a substitution method [7].% * ~ . The hydrostaticvoltagecoefficient gh (dhle&) is also small because of its high relative permittivity k . the piezoelectric phase appears first. VmN-') dh @CP. anumber of different diphasic composites using PZT and passive polymers have been fabricated. the primary goal was to decouple the transverse d3.6 650 30 170 5100 3-2 Perforated 3-2 composite 2. consists of parallel PZT rods embeddedin a three-dimension continuouspolymer matrix [3]. pure. it is evident that the hydrostatic pressure sensitivity of some of the composites was orders of magnitude larger than the corresponding values of the piezoelectric phase used in the composites. Thus. ea is the permittivity of free space. Dielectric and piezoelectric properties of different types of PZT-polymer composite materials designed for the hydrophone applications are summarized in Table I.4 54 40 56 56 27 20 1536 1100 1-3-0 PZT rods-Spurns epoxyglass spheres PZT rods-foamed polyurethane 1. In a diphasic composite.6 1800 2.5 4. As listed in the table. 1-0. Transducers for ultrasonic imaging applications are oper- . for example. The density of the composite could be adjusted between the densities of the component phases. if any. though PZT has a high d33coefficient. From Table I.and 1-3 connectivity pattern. can be minimized. The following criteria were used here to select composite materialof an appropriateconnectivity for a systematic investigation intendedtowards ultrasonic transducers.GURURAJA el ai. : PIEZOELECTRIC COMPOSITE MATERIALS-PART I 483 TABLE I DIELECTRIC AND PIEZOELECTRICPROPERTIES OF PZT-POLYMER COMPOSITES Density (gm/cc) Dielectric Constant K Single Phase PZT 7. By choosingsoftpolymerssuchassiliconerubberand polyurethane. is the key feature in designing the composite materials. A 1-3-0 compositeisa 1-3 PZTrod-polymercomposite with a third phase such as hollow glass spheres or pores not in contact with each other [20]. Itwasshownthatthephase connectivity.5 40 Coral replamine-PZT composite PZT-Spurns epoxy (BURPS) PZT-silicone rubber (BURPS) 3. Composites with porous polyurethane phase were prepared to have positive buoyancy in water. and hence resultsin a better acoustic impedance matching to the human body.5 375 60 200 12000 Description of Composite 3-3 0-3 and d 3 . are large. 2-0. In the notation used here. composites were made flexible.2200 8100 1-3 PZT rods-Spurns epoxy PZT rods-polyurethane 1. Composites of PZT and polymer with 3-1 and 3-2 connectivity patterns have beenfabricated by drilling holes in sintered PZT blocks and filling the holes with epoxy [7].-') dhgh( 1 0 . If the receiving voltage sensitivity of the transducer is enhanced. 3-1. Indesigningallthesecompositemate- g.2-1. The concept of compositetransducerallowsdesigningacomposite structure to enhance the g33 coefficient and improve the sensitivity in the receiving mode. The electrical flux pattern and mechanical stress distribution together with the resulting physical andpiezoelectricpropertiesdepend strongly on the phase connectivity.0 620 450 140 20 45 36 110 180 5040 . In composites most of the PZT (70-90 percent) is replaced by a low-density polymer.3 78 60 41 2460 0. 3-0. 61. PZT is a poor receiver of ultrasound.' ) Reference 100 rials.2-2.

1. The array of PZT rods wasthencastin 10) compared to that of PZT-5 (80). Amongallthedifferentcomposites. Mechanical Q of the composites was low (3to eachother. South Plainfield. The thicknesscouplingcoefficientfor thesecomposites was ers [3].62 339 2. Thus.45 mm rods and with ten and continuous poling technique [23] can be used to polarize 20 volume percent PZT using 0. by Klicker et al.N O. VOL.29 0. such as Fig. This value comorganic binder and then firedat 1285°C for one half hour. A picture of typical compositesamplesisgivenin of the problems encountered in array applications. 484 4.78 1. 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. In brief. 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.55 3 . Table I1 gives long PZT rods. Data for the composite samples used A detailed procedure for fabricatingcomposites with 1-3 connectivity has been reportedby Klicker and co-work. SU-32. [3].onlythose with PZT rods embedded in Spurrs epoxy' matrix with regular periodicity (1-3 connectivity) appeared to be very promFig.28 mm rods.45 0.IEEE TRANSACTIONS ON SONICS AND ULTRASONICS.The 1-3 composites had with silver paint on the major surfaces and poled convenadditional advantages. A N D PIEZOELECTRIC PROPERTIES OF PZT ROD-POLYMER COMPOSITES Rod Diameter (mm) Volume percent PZT ~~ 5 10 0.26 0. ing PZT rods) of PZT rods in each of these composites.anddielectricpermittivity of were chosen for an extensive investigation aimed at high PZT rod-polymer composites have been reported earlier frequency transducer applications.5 mm to 5 ior of these composites might be helpful in resolving some mm. and 30 optimizetheproperties for particular application. Warrington.Thecomposite wasthenelectroded merciallyavailable transducers. 1-3 composites ezoelectric d33 coefficient. the knowledge of the high-frequency dynamic behav. JULY 1985 TABLE I1 PHYSICAL. ten.OS 1.6 375 19 155 I09 I94 238 3 80 94 217 183 1400 ated in a half-wavelengththicknessmodeformaximum sensitivity. Inc. pielements. 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.28 0.in this work are listed in Table I1 along with the properties of single phase PZT-5O1A for comparison. PZT-501A2 rods were extruded using an determined to be about 60-70 percent. Typical 1-3 composites with PZT rods embedded in Spurrs epoxy. The volume percent PZT using 0. PA.45 10 0.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. 20.Because of theseadvantages.73 0.45 0.The composite samples were shaped as circular discs diameter 19 mm and varying thickness from 0. 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 at80°C.1. The pulse-echo amSpurrs epoxy matrix. NJ . minimizing the acoustic cross talk between the adjacent Results on the average properties including density.64 320 2.45 20 Single Phase PZT Density p(gm/cc) Dielectric Permittivity K d~ Coefficient ( pUN) ~ 20 30 Periodicity d (mm) 400 7. Since the composite structure resembles a transducer arof ray.36 - - 0. 'Trademark of Ultrasonic Powders.41 1.78 0.90 1. which can be vaned relatively easily to werepreparedwithapproximatelyfive.28 1. isingfor the ultrasonic transducer application[21]. 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.. Different composites polymer phases. DIELECTRIC. 'Trademark of Polysciences.

the thickness mode. When the composite is used as an ultrasonic transmitter. 2. and the impedance minimum lZ. 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).the loss tangentgoesthrougha peakandcanbeeasilyidentified.fs from the measured value off.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. At the glass L261 transition temperature. which provides a circuitsimilar to the transmissionnetworkrecfrequency. (2) The C. longitudinal and shear wave A . Similarly. the planar mode was thelowest [24]. However.GURURAJA er al. fm andf. BULKMECHANICALPROPERTIES OF SPURRSEPOXY Radial Mode in Spurrs epoxy is the piezoelectricallyinactivephase thecompositematerialconsideredhere.Knowledge of the resonant vibration behavior of the composites in air is important and helpful in the evaluation of the composites as anultrasonic transducer operating intowaterequivalent load. and a number of lateral modes related to the regular periodicity of the PZT rods in the composite.5 MHz. P V. A spectrumanalyzer(HP 3585A). C . as illustrated in Figure 2(a).: PIEZOELECTRICCOMPOSITEMATERIALS-PART 485 I _--. In a circularly shaped 1-3 composite material. vibration behavior of the composites are presented here. and&. The glass frequencies fm and f. TR was found tobe a functionof frequency varying from 70°C at 1 0 0 Hz to 121°C at 1 MHz with a shift of 12-15°C per where the figure of merit M is given by decade of frequency. Only the results which are useful for analysis of the frequency resonance mode. the geometric tenuation of the transversewave in Spurrs epoxywas measured to be 6 dB/cm at 0. These properties of the polymer dedisc. and R .l at rescient wasfound to increase with thesquare of the onance. the epoxy has to effectively couple the ultrasonic energy fromahigh-acoustic-impedance PZT to a low-acousticimpedance load.capacitance C. corresponding to minimumand maxtransition temperature is defined as the temperaturebelow imumimpedance.. In the present Standard recommends the following approximation to calwork Tg and its dependence on frequency was determined culate Af = fp . are quitedifferent fromfs and&.theresonancemodesobservedare theplanar mode. Planar-ModeResonance velocities.Characterization of thedifferentresonance modes in 1-3 PZT rod-polymercompositewillbedescribed in thefollowingsubsections. which was measured at a frequency well below fundamental resonance.ForSpurrsepoxy. The atand parallel resonance frequenciesf. RESONANCEMODES 1 Resonance modes in composite materials.(a) Radial mode.27 X lo6 kg/m2-s. as in single phase materials. TheIRE thematerial is rubberlike andsoft [25]. IV. The acoustic impedance of the Spurrs parameters for calculating these constants are the series epoxy was calculated to be 2. and f. The glass transition temperature Tg is another ommended by the IRE standard. its function in thecompositetransducer is quitecritical. These approximations are valid for resonances with M > 3. The sum (C. C . 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. importantparameters of thepolymerthatinfluencethe performance of the composite as an ultrasonic transducer are its acoustic impedance. respectively. The most important m/s. In thepresence of highmechanical which the material behaves like a glass and above which losses. The Fig. was used in measuring characteristic parameter for polymeric material. The planar coupling coefficient kp was calculated from the expression given by [27] + l + a 1 . is the resistance of the series branch of the equivalent circuit of the piezoelectric material near resonance. The attenuation coeffi. are defined by the geometry and dimension of the specimen. for instance at 1 KHz. 1 2rfJ1Co M = I 2nfm(Co + CI)lzml. (b) Thickness mode. ) is the static capacitance. electric field in the 3 direction composite.and attenuation coefficients and their depenThe planar mode (alsocalledradial)vibrationinthin dence on frequency. are the capacitance of the parallel and series branch. in the receiving mode. Resonance modes in a disc-shapedpiezoelectricmaterial.. the ul(b) trasonic energy incident on the composite shouldbe transferred effectively to the piezoelectrically active PZT. by measuring the dielectric loss tangent of Spurrs epoxy as a function of temperature and frequency.

Theeffectivemodulus by the Reuss model is given by _1 -. The modulus E. fs was measured and D was assumed to be 0. and Q is of the sameorder.5 1.. This assumption seems appropriate for a combination of hard filler in a soft matrix. SU-32.lp)”* corresponds to the longitudinal velocity C. As it emerges from Table 111. by obtaininganexpression for the elastic modulus E. (3) and ( 5 ) used for calculating kp and Q are not fully valid for values of M < 3. of the composites increases with increase in the volume .0 3626. from (6). the figure of merit M for the radial-mode resonance of all the composites was between one and two. p is the density.3 as already mentioned. A similarexplanation can be given for the difference in the frequency constant between the thick and thin samples.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 Q 0.5 34 1.0 1.6 1.1 18.IEEE TRANSACTIONS ON SONICS AND ULTRASONICS. 6 mm.3 26. The f. NO. Subsequently. and a is the radius. was calculated from the expression C. The value of R1 = 2.4 34 1561 1409 1506 l33 1 1454 1324 1458 1439 1529 1352 1474 1046 ‘Thick = 0 . (4) was simplified to fraction of PZT. JULY 1985 486 TABLE 111 ELECTROMECHANICAL PROPERTIES OF COMPOSITES FROM THE RADIALMODERESONANCE Volume percent PZT (Rod Diameter) Thickness’ 5 (0.C?)]”* where fs is the series resonance frequency of the planar resonance._U1 + -“2 Et E.5 to 2. 0 1.11. An attempt was made to theoretically estimate the longitudinal velocity C. However.1 22.1 42 1.0 21. the uncertainty in assessing k.45 mm) 30 (0. C. was approximated tofm.6 consisted of thinsampleswithathickness mm. The frequency constant Np for the planar mode (product of resonancefrequencyandthediameter)isalsolisted in the table. the Poisson’s ratio of the composite was assumed to be 0.45 mm) 20 (0. 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. Knowing E. Hence the results can be used for a relative comparison of samples having different volume fraction PZT.5 1..Thesecondgroup was comprised of allsamples thicker than 3 mm and was classifiedas thick samples. becalculated by theReussconstantstressmodel which assumesthat the two phases experience equal stress. 40 17. Since the Poisson’s ratio of both PZT and epoxy are approximately 0. in the transverse direction can [14].8 23.lp(l 27ra The calculated values of kp and Q from (3) and ( 5 ) for several composites are summarized in Table 111. perpendicular to the rod axis as a function of volume fraction of PZT.3. and thin > 3 mm. 02 3 . is the elastic modulus of the composite perpendicularto the PZT rod axis.05 for U = 0.3. perpendiculartothelength of therodislisted.1 20.45 mm) 10 (0. VOL. = (E. As mentioned before.97 . Thecouplingbecomesmore efficientforthicker samplesindicating a greater homogeneity. In calculating C.0 25.45 mm) l0 (0.5 to 2 . Table I11 indicates that the planar coupling coefficient k. The first group investigated of about 0.05 [(E. In ( 6 ) (E.. The mechanical quality factor Q can be evaluated from the relation [26] For M > 3. because the matrix should deformmorethanthefillerandthestressinsuchasolid shouldbefairlyconstant.1.2 23 21./fi)”2.0 1. perpendicular to the rod axis. Thick composites have a higher kp comparedto thincomposites of thesame volume fraction.28 mm) 20 (0. 4. The properties remained virtually constant in the two extreme limits. the valuesof kpand Q listed in Table 111 are far from being exact. In the last column of Table 111. The data listed in the table are an average of the measurements of at least five samples.28 mm) Thin Thick Thin Thick Thin Thick Thin Thick Thin Thick Thin Thick M k.was calculated using the relation [27] fs = 2.7 36 16. and the density p of the composite (Table 11). the longitudinal velocity C. since the value of M is approximately the same for all the samples. E2 (7) .. where U is the Poisson’s ratio of the material.72. The effective modulusE. The data are divided into two groups depending on the thickness of the sample.3. The value of C.

the amplitude of the resonancespectrumdecreasedgradually with temperature andwassuppressed below 0. The planar-mode resonance was studied as a functionof temperature up to 100°C. 487 ness decreases. : PIEZOELECTRIC COMPOSITE MATERIALS-PART 2300- I I l I 1 - - l300 0 I IO I I 20 30 l 40 50 Volume Percent PZT Fig. (50 KHz).GURURAJA er al. Measurementscould not be made on the radial-moderesonance above 100°C. approaching the Q of single-phase PZT 501A (80) [28]. It is conceivable that the suppression of the radial mode above 100°C is due to the very lossy nature of the Spurrs . Longitudinal velocity perpendicular to the PZT rod axis as a function of volume percent PZT In composites. It was observed that the planar couplingcoefficientremainedvirtuallyconstant with increase in temperature. However. 3. Itis interesting to note thatthis temperature corresponds to the glass transition temperature of Spurrs epoxy (Section IV) at the resonance frequencyf.1 dB at 100°C.

820 1. dard method was used to calculate these properties of the It is also known that the Spurrs epoxy is extremely lossy compositecorrespondingtothethickness-mode reso.6 dB/cm).225 2.5 to three times larger ure of merit M for the thickness mode resonance than the separation distance between the PZT rods in the othersampleswasabovethree.9 2.15 fm IRE .tenuation of the transverse waves in the epoxy is relatively mined by the vector impedance method on a selected num.transverse wave velocity to be 1150 m/s from Section IV). thefig.For thicksamples (due to theelectrical excitation) and the mechanical inter( t > 3 mm).8 30.60 5.54 3.4 Vector Impedance Method Method Kp (%) Q 24 22.and Q was three to ten. VOL. and frequency constant compared to composite.45 mm.3 1.6 27.verse wave must be significant to cause a strong interaction between the rods through the epoxy medium. PZT rods vibrate with a large amplitude.8 0.9 48 20.6 39 22.5 MHz and the The thicksampleresonatearound thickness above 3 mm. withthickness around 0. In the first approximation the interaction is assumed to involve only nearest neighbors.f. with the exception of the five percent PZT composites.760 2. The low mewas 20 to 30. In thick thick samples both k.05 3.320 1. PZT rods. At the resonance frequency.168 1.929 37 24.2 2. The couplingcoefficient and the frequency constant of thin sampleswereclosetothat of single phase PZT = 3700 Hz m for PZT 501A (k33 = 70 percent. 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 0.7 1.8 Q 39 37 37 'In a 20-percent PZT composite.waves generated in theepoxy interact with the array of onance of 1-3 composites.5 MHz ( .IEEE TRANSACTIONS ON SONICS AND ULTRASONICS. These transverse Fig. with rod diameter = 0. the amplitude of the transber of samples were within two percent of the values cal. Indeed the values of the kt and Q deter. the wavelength of where r is the thickness. The low culated by the IRE standard method.842 1.5 mm (taking the terms in (8)-(IO) is given in Section V-A. Effectiveness of the interaction depends on the amplitude and phase of the and transverse wave relative to that of the PZT rods.of the phase cancellation effect betweenthe vibrating rods 70 percent.41. The wavelength is 1.81.364 1. Theexperimentalresultsaresummarizedin Table V.48035 35 21. Since the atand Q are valid.041 1. 4.585 1.low at 0. SU-32.0 1.for transverse waves at this frequency.6 mm).25 MHz.and Q action between the rods through the epoxy. composites of different volume percent PZT.1 1.79230 fp -fs kp (%) 0. coupling coefficient in thick samples is probably a result Datalisted inTable Vindicate thatforthethickness mode resonance of thin samples (r = 0. The IRE Stan. Af= fp -L (KHz) M (KHz) 2.998 2. andthemeaning of theother the transverse wave is approximately 0. The relatively low Q of thin samples indicates The data are again divided into two groups: thin samples that the rod vibrations are partly damped by the surrounding polymer. 4. The observed behavior of the composites in thicknessmode resonance can be explained as follows. and NP were proportional to the volume percent of PZT.66 2.386 2.wavelength of transverse waves in the epoxy is approxiof all mately 2. e .350 72 12. thin composites had higher coupl-chanical loss in the epoxyis reflected in the high Q of the ing coefficient k. thick samples while the mechanical Q showed the reverse trend.0 2.172 1.Hence. In general.theapproximationsrecommended by the IRE Standard to calculate k. This results in only a weak interaction between the vibration of neighboring nance. k. NO.95 4. ' C perpendicular to the axis of PZT rods. was approximately 50 percent. PZT rods. For thin Np = f p t (10) samples resonating around 2.184 43 22.3 mm. As it can be seenin the table. Effectof temperature on the Frequency constant of radial mode res. kt was 60.6 mmandthicksampleswith 0.711 27.9 25.and 501A) and were independentof the volume percentof PZT.7 26. The vibrating rods act as a source of complex trans5 0 0 0 " " " " 50 " " " ' l00 I50 verse waves intheepoxypropagatingin adirection Temperature.

the calculated values in Fig.propagation 40001 I 1 I I 1 .6 4 22 1956 1403 2912 2806 20 0. The behavior of the composites could be explained by stant electric displacement).0 7 23 1820 1492 3640 2984 20 (0.45) 0.45) 0. these resonances always ocwhere El and E2 arethemoduli.9 9 1603 18 55.6 40. and A2.1 27.1 1853 3706 3203 2.4 5-7 72.2 5 c. AI. 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). E ~+ u ? E ~ (11) For a certain volume fraction. Lateral-ModeResonances In additiontotheradial-andthickness-moderesonancesandtheirovertones.5 31 1834 1327 3668 2654 10 (0. The frequencies of these resonances were independentof sample thickness. A Brillouintheory of elastic wave supports the equal strain model for calculating the effecin a twodimensionallyperiodiclatticecortivemodulusofthecompositealongtherodaxis. The resonances at&. El = u .0 5-7 50. 5.and u I and u2 a rethe curred at specified frequencies regardless of the thickness volume fractions of the two phases (PZT and epoxy). calculated usingtheformula Cl = 2tf. In the vicinity of the resonances of A.6 3.28) 0. The comcomposites of different volume fractions. The resonance corresponding to fi was inversely proportional to the thickness of the sample.0 8 25 1874 1555 3748 3110 1.4 12 61. For of the sample. Such behavior suggests that resonance at fi is the modulus EI of the composite parallel to the PZT rods.6 2.GURURAJA er al. percent Q 5 (0. A2 as categorized in Table VI.45) 0. The longitudinal velocity wavelength is much frequencieswherethetransverse of sound.major resonances of interest are designated as fi.6 3 to 5 5-7 5-7 68. Longitudinal velocity along the PZT rod axis as a function of vol. As can be seen in Table VI. The longitudinal velocity Cl simpleaveragingschemessuchastheconstantstrain was calculated from the relation Cl = (El/p)"2.5 x 10" N/m2(the Young's modulus of the rod at con. the very well withthetheoreticallyestimatedvalueforthe Voigt constant strain model [l41 can be applied.9 (0. agrees larger than the separation distance between the rods. 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. At longitudinal thickness vibration.6 4 to 6 2. 2NP 30 - - - - - - (0.1 26 1687 3374 10 (0.0 40.28) C. 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. 5. The experimentally determined longitudinal velocity Cl.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. and ume percent PZT in composites. as discussed in posite modulus using the Voigt average is written as detail in the previous section. but were related to the lateral periodicityof the PZT rods in the composite.6 3-5 3. increase in the PZT rods witha diameter that is small compared to length.6 62.9 to 3.higher frequencies. is given in or small compared to the lattice periodicity (Section V-A the last column of Table V.45) 2.: PIEZOELECTRIC COMPOSITE MATERIALS-PART I 489 TABLE V THICKNESS-MODE RESONANCE I N COMPOSITES Longitudinal Frequency Velocity Constant Nf (Hz m) (mis) Volume Percent PZT (Rod Diameter in mm) Thickness (mm) Figure of Merit M k.6 4-6 4-6 68. 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. model and the constant stress model forwavelengths large expressed as twice the frequency constant @. Three Fig.4 57. and&? were very similar in nature. This velocity is compared with and V-B).otherresonanceswereobserved in the frequency range 0-2 MHz.

a similar standing wave solution along y also exists. constructive reflection (Bragg-scattering)occurs fromverticalplanes of rods. = dfil c 3 (1 = -r v2 51 52 53 54 0. Unit cell geometriesandlaserscanpaths.00 4. so that resonant scattering of the x-propagating wave into a y-propagating wave occurs.45 2.45 0. but there is n o resonant scattering into y-propagating waves.5" to the x and y axes.45 2.27 1.spaceharmonics are generated but none are resonant. Relativeamplitudeand phase of the ultrasonic displacement was measured along two scan paths: along a row of PZT rods and on the epoxy surface in betweentwoadjacentrows of PZT rods as . Here the rods all vibrate in phase and correspond to the second stopband of the square lattice. The samples were fine polished (+ 1 pm) andelectroded with highly reflecting gold electrodes for the laserprobemeasurements.73 0. As a result.58 1. the solution is a two dimensional resonant standing wave pattern as shown in Fig. However.Thesey-propagating waves also experience resonance scattering of the same type. 4.OS 3. butin this case.54 3 . (a) Standing waves at the second stopband. a spatial modulation of the phase fronts is produced by the difference in the properties of the rodsandmatrix.A t the stopband edge. detailed laser probe measurements of the actual displacement on the composite to analyzethenatureofvibration atthesefrequenciesarereported.andresonanceoccursbetween adjacent vertical planes.80 5 .45 0.90 0.44 5. . in 1311.the lowest stopbandfrequencieswerecalculated. Similar conclusions areobtained forz-propagating wavesof otherpolarizations.Consequently. LASERPROBEMEASUREMENTS The measurements of actual displacement on the composite samples were performed using the laser heterodyne technique [31].76 1.90 0. x-propagating shear wave is incidect on the grating. respondingtothe PZT rod-polymercomposite was developed by Auld er ul.45 0. alonr the unit cell diagonals.45 0.15 0. SU-32. 6. = 2tfi - 730 - - - - 8782330 2496 25 l4 908261 8 954 853 790 769 h 859 - - - - - When the rod spacingd is one'shear wavelength.90 0. VOL.64 5. This behavior corresponds to the first stopband of the lattice.5 1125 1188 - 2778 2848 82 1 867 Scanned obng rods - (a) (b) Fig.93 3. in KHz Percent Volume 5 10 20 20 30 30 Rod Thickness I Periodicity c. h. The x-propagating wave is also scattered from planes of rods at 4. NO.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. The essential phenomena can be explainedby reference to Fig. 6(a). 6(a).45 2.90 0. x-propagating wave is again Bragg-scattered with a phase shift of 27r from one vertical plane of rods to an adjacent plane. Bragg conditionsare not satisfied A stopband exists at d = and resonance does not occur. However. it is easily verified that the wave is also Bragg-scattered at the same frequency by the 45" planes of rods. From the square symmetry of the lattice.76 437 450 3I2 262 222 483 449 101 I02 103 0.45 0.45 0.45 0.60 5. 6(a) that a z-polarized.95 4. (b) Standing haves at the second stopband.45 0.73 569. illusas trated in Fig.76 1. JULY 1985 490 TABLE V I R E S O N .Theexistence of stopbands was related to Bragg-scattering from planes of rods having various orientations in the square lattice. a completely different standing wave pattern results.90 604 1.45 1. along thc unit cell edge.15 0. In the following section. the solution is a standing wave along x. In this case a z-polarized.27 1. Suppose in Fig. 15 I .IEEE TRANSACTIONS ON SONICS AND ULTRASONICS. 786 691 c. 6.). no Bragg scattering can occur because the structure is uniform along z . Forlaterallypropagating shear waveswith polarizationalongtherods.5 276. For-a z-polarized z-propagating wave incident on the lattice. ~ NMODES T IK COMPOSITE M A T E R I A L S Resonance Frequency . VI.45 0.59 4. At a frequency for which the rod spacing d is one-half the shear wavelength (X./2 for an x-propagating wave.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.

The composite vibrates uniformly across the surface with almost equal strain on Atf2.311. which corresponds resonance along z. (Vibrations at the first stopband discussed earliertheperiodicity of thelattice. Because of symmetry. 6(b) that the displacement at point d . The only variable in the samples 8(a) and at the equivalent point in Fig. 10. The PZT rods vibrating due tively. possibly duetoimperfections in resonance frequency.and there is no noticeabledifference in amplivibrate in phase and can be excitedby uniform electrodes. 8(b) are less sat.are the wavelengthsof transverse wave at thethickness isfactorilyreproduced. The difference in amplitude of vibration between the PZT andepoxyobserved in sample 101 is greatlyreduced in B. waves illustrated shows that the z-displacement has a posFig. 7. (Fig.. 9 shows the complex vibration pattern length of transverse waves in sample 102.andthishasbeen verified experimentally.)Superposition of the x and y standing expected to be more uniform. The 4.Thevibrationpattern than that predicted from the assumed standing wave pat. In the scans of Fig.4TERIALS-PART er al. Fig. 10-12 compare the ultrasonic displacements on the itive maximum at a .0 mm. as predicted.9. 102. 9. C .sampe 101 are not measurableforsample ments at a and b. 6. and maximum in phase displace.: COMPOSITE PIEZOELECTRIC 49 1 I - 40 predictedtobezero. of transverse waves.ultrasonicdisplacementonthecomposite is trodedsample. Thisispossibly due to the mass loading by the PZT rods. simple sinusoids. thickness = 1. standing transverse waves along the unit cell diag180" thePZTandepoxy. and zero at surface of composites 101.27 mm. These features are clearly observable in probably because of the reduced attenuation in the epoxy the scans of Fig. so that weaker standing-wave patterns are to be plane. period = 1. which are respectively 1. The vibration pattern depends very much along the unit cell. 6(b). 8. for this sample. Vibration Pattern at Frequency f.93 mm).45 mm. The transverse waves produced inThe plot in Fig. is This uniform ultrasonic displacement observed on the sur- A . It thickness ofhomogeneous the plate was noted earlier that no resonant space harmonic exist in this case. Transducer diameter = 19. when transverse wavelengths are large compared to periodicity. is clearly visible inthe figexpected in the ure. = dfil is tabulated in transverse wave velocity in Spurrs epoxy of1150 m/s). 2. Vibration Pattern at Frequency f( 400 IO00 Frequency ( K H z ) I600 Fig.. ticeequal to 1. 8 shows the complex vibration pattern teract with neighboring rods to produce the resultant viatfrequency 5.7. to electrical excitation act as the sourceof transverse waves in the epoxy travelling in a direction perpendicular to the axis of the PZT rods. The small phase variations are attributed to the damping in the composite which was not considered in the theshown in Fig.GURURAJA M.PZT rod diameters = 0. The predicted zeros at c in Fig. the amplitude of vibration showing the existence Of three strongresonances.energy from PZT to epoxy. This is attributedtothepresence of higher space tion in Section V-B of the constant strain model used to harmonicssuchthatthestanding wave patternsare not calculate the effective modulus along the fiber axis. 6(a)). and 270 KHz. It can also be seen from Fig. midway between a and b . 7 giveselectricalinputimpedanceory outlined above .thesestatements applyatall nating in the longitudinal thickness vibration at frequenequivalent points in the lattice. 10 shows plots of complex vibration pattern at the the to simple longitudinal frequency fr. respec. For sample 103 at frequencyj? corresponding to the stopbandin Fig. Measuredelectricalinputimpedance of compositetransducer #l01 (tenpercentPZT in Spurrsepoxy.3 mm for the above three samples (calculated using the velocity of the transverse waves. Vibration Pattern at Frequencyft2 sample 102. the cies 620.27 mm. All the samples maxima of the standing wave pattern at a and b arel80" have ten-volume-percent PZTwith a periodicityof the latout of phase. . c. negative maximum at b . This is directly attributed to the longer waveThe plot in Fig. on the epoxy at f i is about 5 to 8 dB larger than on the show laser Scan plots Of vibration amp1itude Figs' PZT rods indicating an effective couplingof the ultrasonic and phase taken at frequencies f t l .periodicity. and 103(Table VI) resoc . andfi. except that the maximum ata is smaller atlowerfrequencies(SectionIV). This is out of phase at a and c . the transverse wavelength is more than three times the peThis is another of the higher stopbands for which the rods riodicity. tude between the PZT and epoxy.observed in sample 103 is in accordance with the assumptern. 414. where the rods all vibrate on the wavelengthof the transverse waves in relation to in phase.Smallphasevariationsseenacross onals are superposed to give maximum displacements 103. As the wavelengthof the have a 180" phase shift from one plane of the rods to the transverse waves becomes larger compared to the lattice next and cannot be excited electricallyin a uniformly elec. respectively. Table VI. data taken On One Of these lol in As is clearly Seen in Fig. correspondingtothesecondstopband bration pattern. Fig. and the lattice and inaccuracy in alignment of the scan. The velocity C. as tabulated in the last two columns of Table VI is lower than the measured velocity of 1150 m/s (Section V).

Sincethe acousticimpedance of the epoxyis relatively In this section the effect of temperature on the electroclose to that of the human body. EFFECTOF TEMPERATURE face of the composite is a clear indicationof efficient couRESONANCE M ODES pling of the mechanical energy from PZT to the epoxy. JULY 1985 D e I (mm) -Position (mm) -60- - Position ON THE VII.SU-32. It is clear from the preceding sections that the high-frequency man body is ensured.IEEE TRANSACTIONS ON SONICS AND ULTRASONICS.mechanical properties of the composite is discussed. . 492 4. an effective coupling of acoustic energy from the composite transducer to the hu.NO. VOL.

(a) Scan along rods. Thus. the resonance behavior of composites freely suspended in air was studied as a function of temperature from 0 to 150°C. Laser scan measurements of relativeamplitudeandphase of the acoustic vibration atfr = 620.I l dynamic behavior of 1-3 composite is strongly dependent on the mechanical properties such as the velocity and attenuation of ultrasonic waves in the Spurrs epoxy. having a wide range of elastic properties.7 KHz (sample # 101). mechanical Q. IO. In the experiment. The Spurrs epoxy is glassy at room temperature and goes through the glass transition temperature to a rubber likematerial in a temperatureinterval ofonly about 100°C. These properties of Spurrs epoxy are very sensitive to temperature. 103 (ten-percent PZT compositewith .Intheglassystate. Fig.GURURAJA et a l . The thickness-mode coupling coefficient k. and the frequency constant N f of the composite were determined at 2°C intervals both in heating and cooling cycles. : PIEZOELECTRICCOMPOSITEMATERIALS-PART I 493 " 'c 'Or 15 S i Fig. it was also shown(Section V-A) that the compliance of the epoxy increased by approximately 65 percent in the temperature range of 0 to 100°C.1 to 1.45-mm rods. The heating and cooling rates were maintained at approximately 2"C/min. 13 shows plots of absolute value of admittance as a function of frequency from 0.1 MHz for sample 0. a study of the temperature dependence of the resonance modes will help in understanding the elec- tromechanical propertiesof composites with different polymer matrices. (h) Scan between rods. ..

It may be reeventually disappears ata temperature around 135 "C. JULY 1985 Fig. the amplitude Thebehavioris typical of allthick(thickness > 3 mm) mode was increased (Fig. the epoxy is rubber like and soft. the mechanical interaction among PZT rods through the epoxy resonancefrequency AI. and Q of the thickness-mode resonance for sample 130 are plotted as a function of temis denoted byf. 13. k.262 transition temperature.In the temperature effect. In the 3) Resonance at 1. This resonance is denoted byf. 13(a)) were identified as follows. rate than the resonance frequency fi.6 mm) composite disappearance can be attributed to the fact that above the sample. 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. (b) Scan in between rods: of thickness thickness 5. and Q was 3-10 (Table V).644 MHz was identified as the stand. after the transverse mode had disovertone of the thickness mode. k. gradually approachesf. The effect of temperature on the above resonance modes The observed coupling coefficient k. was 60-70 percent.. The value of k. respectively. which is defined by As a result. (a) Scan on rods.perature in Figs. As seen in Fig.at becomesweaker as also indicated by an increase in the higher temperaturesf. which is mainly determined by matrix. f r l passesthrough h and the damping provided by the lossy polymer. . and finally amplitude of the resonance spectrum (Fig. At temperatures above the glass transition temthe elastic modulus of the polymer. As the temperature was increased from 25"C. changesubstantiallyuptoapproximately110°C.bles that of a thin composite at room temperature. the epoxy is expected to me. Therefore.. from Section IV). decreased at a faster perature TK = llO"C). the mechanical Q at 25°C was about thickness-mode resonance were ascribed to the overtones 20. the mechanical interaction among PZT rods thecompositemodulus E. 13(b)-(d).15 mm) at different temperatures up to 170°C. NO. the two modes interferewith each other.494 IEEETRANSACTIONS ON SONICS AND ULTRASONICS. of the composite approach kS3 of afreely susrange 11O-13O0C. 13(e)-(h)). 14 and 15.. exhibited a minimum. The secondary lowcomposites. at approximately 110°C. (0. increasedsignificantly to about 60 percent. 13(e)-(h)).sample at room temperature were attributed to the strong chanically soften at a faster rate than PZT. the three major resonances observed at room approximately100°C. 12.It appears that the wave (glasstransitiontemperature of Spurrs epoxy is nature of vibration of a thick composite above TK resemaround 110°C at 200 KHz.Thisdisappearance is againastemperature (Fig. Above 130"C. It is worth. Laser-probemeasurements of relativeamplitudeandphase of the acoustic vibration at pi = 270 KHz of sample #103.030 MHz was identified as the third temperature range from 100 to 130"C.) is explained by the following. 15. 2) Resonance at 0.frequencyresonancesclearlyseenat25°Cdisappearat vious section. SU-32. Weak secondaryresonances below thefrequency of appeared.48)determined atroom temperature(25°C)did not ing wave pattern in the epoxy arising from lateral periodicity of the PZT rods. In merges withf. 4.. k. VOL. cribed to the lossy nature of the epoxy around the glass MHz was identified as ahalf 1) Resonanceat0.Accordingtotheanalyses given in thepre. The Q remained constant to approximately 100°C and of the planar-mode resonance of the composite disc. and Q in a thick (Fig. k. while to note that above 130"C. This called here thatfor a thin (thickness = 0.. decreased to a value of five at temperatures above 130°C. pended PZT rod (70 percent) and Q decreases because of At temperatures above 130"C. wave resonance along the thickness of the composite and The coupling coefficient k. As shown in Fig.

l MHz and the y axis is the relative admit!.1 t f l 1 . 495 .ance (50 dB). The x axis isthe frequency 0. Temperature-dependenc e o f various resonances in a composite samples (sample # 103). 13. : PIEZOELECTRICCOMPOSITEMATERIALS-PAR7 (d) I (h) Fig.CURURAJA e1 al.

” Muter. vol. versus I?] -.1978. 14. NO. Bull.. Res.Whenthisconditionissatisfied.. Cethickness mode frequency at 2.. Mrs. LindaWebsterforpreparingsamples. perature above TR is unlikely to affect the resonance behavior. cc 0. 4. The experimental results werein excellent agreement with the theory of wave propagation in two dimensionally periodic solids. Newnham. D. J. k. o Cooling Run H e m n q Run ACKNOWLEDGMENT -7 The authors are grateful to Dr. E. From the effect of temperature on resonancebehavior. For a givenvolumepercentPZT. 599-607.S U-32. For thickness mode resonanceof thin samples. additional modes were observed because of the regular lateral periodicity in the structure. E. 1978.13. dence of the electromechanical properties of composites is very weak at room temperature. Moses for writing software for computer interfacing. V. “Piezoelectric comture range of 0 to 150°C. Cross. A. was seen over the entire tempera141 K. Soc. C208-C210. 16). For thick samples. coeffi- REFERENCES In thin samples.” Marer. Shaulov of North American Philips Laboratories and Dr. 1 IO0 200 0 0 Temperature. ‘C Fig. of Electrical and Computer Engineering and Biomedical Engineering and ScienceInstitute) for theircommentsanddiscussions. 5-8. A . W.” J.CONCLUSION The resonance modes in circular shaped 1-3 PZT rodpolymer composites were fully characterized.” J. nificant variation of k. the increase . Klicker. V.thecompositevibrates like a homogeneous body and it will be shown in Part I1 of this work that the composite materials exhibit excellentsensitivity operating into water load. Compositeswith low transverse coupling could be utilizedforlinearand phased array systems. the planar coupling coefficient increased with increase in volumepercent PZT. Newnham. P.25 MHz (Fig. Amer.and R . No sigrum. 64. A . “Flexiblecompositetransducers. In general. vol. At the thickness-moderesonance. and J. This seems to be confirmedby the plot of k. 1982. temperature for a typical thincompositesamplewith 131 K. Schulze. it is clear that theinteractionamongthePZTrodsthroughtheepoxy matrix can either be enhanced or suppressed depending upon the properties of the polymer phase.IEEE TRANSACTIONSON 496 SONICS ANDULTRASONICS. 13.6. Smith and Dr. Lewin of Drexel University (Dept. 525-536. ~01. pp. W. Klicker. A. Biggers. Skinner. VIII. thick samples had better planar coupling coefficient than the thin samples.“Composites of PZT and epoxy for hydrostatic transducer applications.. the temperature depenposites with 3-1 connectivity and a foamed polyurethane matrix. = 6070 percent and Q = 3-10. A .pp. vol.andMr. 1981. The difference in the observed behaviorwasexplained by considering thestrength of the interaction among the PZT rods through theepoxy. pp. P. Soc. Res. Typical effect of temperature on the thicknecs coupling coefficient of a thick composite sample (sample # 103). Thus. P. kt = 50 percent and Q = 20-30. Biggers. when the transverse wavelength in epoxy at the resonance frequency was much larger than the periodicity of the lattice. A . The resultsshowed that these resonances arose from the superposition of the standingwave pattern of the transverse waves in the epoxy. VOL. Typicaleffect of temperature on thethicknesscoupling cient of a thin composite sample ( I ) .and L.60 50 l00 I50 Temperature. JULY 1985 further supports the proposed model describing the nature of vibration for different resonance modes of 1-3 composites.pp. Bull. Cerum. In addition to these two modes of resonances. since the coupling among the PZT rods [ I ] R . 16. E. “Connectivity and of tempiezoelectric-pyroelectric composites.thecoupling of acousticenergy from PZT to epoxy was found to be most efficient. “ C Fig.Arner.

pp. Dr. SU-26. vol. second harmonic generation. McGrath.piezoelectric. Robert E.A.” IEEE Trans. pp. i n 1956 and subsequently he receivedthe Ph. India.degree from Colorado State University. Jap. Schulze. E.andcompositematerialsfortransducerapplications.“Ultrasoundtransducersfor pulse-echo medical imaging. Auld. N. pp. part A. 50. 453-481. Banno. vol. and J. MA. 171 A. A. 1979 /€E€ Ultrason. 407-411. 47. and H. L.Ross. 497 T. in 1952. Sonics Ultrason. vol. pp. Lynn. [l21 C.” IEEE Trans.” / E E E Trans. 41. [21] T. R.ceramics. 1983 /€E€ Ulfrason. 1948. 1969. London:Academic.Safari. He is currentlyAssociateProfessorwiththe Ceramic Science department at Alfred University. 191P. E n g . M.and W. 955-958. Schulze. IRE.andpyroelectricmaterialsandcomposites. 13-20. vol. and G. [26] “IRE standards on piezoelectric crystals: Measurements of Piezoelectricceramics.L. Schulze hasbeenworking in theareas of ferroelectric. 1929 in Amsterdam. Goll.“Per- foratedPZT-polymercompositesforpiezoelectrlctransducerappli- cations. vol. 1980. . 1983.P. 115-125. Cross (SM’79-F’84) was born on August 14. Shui. W. Wilson.” Ferroelecfrics. vol. 67-69.Schulze. 1981. 39. L . he is Professor of ElectricalEngineeringandAssociateDirector of the Materials ResearchLaboratoryatThePennsylvaniaState University. 197-205. Schulze. The Pennsylvania State University. and I.andL.HereceivedtheB. pp. A ..D.” in J.” IEEE Trans. Holt.“Piezoelectricanddielectricproperties of composites of syntheticrubberandPbTiO?andPZT. He is alsoworking on ultralow permittivity materials for packaging Ga:As integrated circuits. Kanpur in 1978 and the Ph. A . EerNisse. A .and Y. “Piezoelectricity in polyvinylidene fluoride.” IEEE Trans. Rev.D.“Electrostrictive effect in bariumtitanateceramics. “Piezoelectric and piezomagnetic materials and their function in transducers. Cross. Fraser. A.49. Kunkel.” in Proc. J. E. D. pp. New York: Academic. Auld.andF. T. Cambridge. Foster. Prior to joining ThePennsylvania State University. 1977. Saito. S . Y. Gururaja. 74. S. vol. degree in materials science from the IndianInstitute of Technology.P.pp. “Recent measurementsonimproved thick-film piezoelectricPVDFpolymermaterials of hydrophoneapplications. 554-558.D.and M.S.dielectric. degree in physics from The Pennsylvania State University. 222-225. and L. Leslie E.. Newnham aDr. K. [29]C. E. vol. He received the M. and electrical property measurements.. 1141 S." J. 52-53. Curran. 385-393.” IEEE Trans. in physics from the University of Mysore. A. 1134-1147. R. [l31 J. R. “Multilayer impedance-matching schemes for broadbanding of water loaded piezoelectric transducers and high Q electricalresonators.“Accuratemeasurement of coefficients in a ferroelectricceramic. University Park.. “Design of low-loss widebandultrasonictransducersfor noninvasive medical application. 1983. SU-24.. Klicker.“Stress wave propagation in compositematerials. 1983. Hunt. Soquet. W.andcomposites. in 1974 and 1976.. P. K . “Ultrasonic measurement of some minera1 filled plastics. D. vol. Before he joined The Pennsylvania State University. 93-106. He receivedhis Ph. Kino. CurrentlyDr.GURURAJA er a ! . He worked as Senior Research Associate at The ’ Pennsylvania State University from 1974 to 1983. W. . m”: currently isHeResearch Associate with the Materials Research Laboratory. pp. R. Sonics Ultrason. vo1.“Transmitterand receiverformedicalultrasonics. [l11 J. SU-25. Y.20-30. 1981. K. Newnham.A.SU-22. vol. pp. 1979.“Bulkmechanical properties of the Spurrs epoxy and eccogel polymers. He is also the chairman of the solidstatescience program. I _- > . “Thedesign of broadband fluid-loadedultrasonictransducers. [22] K.” IEEE Trans. 1978. Sonics Ultrason.SU-26. 1982.pp. L.andPh. Webster. He received the B. T. Newnham.Newnham is Professor of solid state science and ceramic science at The Pennsylvania State University.Ferry. from 1958-1966. “Compositepiezoelectrictransducers. 1966. Symp. D. A. Rlttenmyer.ceramicsand composites. [24] T.thick-filmmaterialsforcircuitryanddielectrics. 173-181. degree from Hartwick College. 1964. Hisresearchinterestsincludeferroelectricmaterialsandferroic phenomena. His research interests include crystal physics and structure-property relationships. ”‘g. Newnham. A. He is author of a bookentitled StructureProperty Relations. [l51 J. and C. Jones.Safari. Newnham was born on March 28. D. E. A. T. W. 1979. M. University Park in 1984. Fort Collins. [l71 J.. H. pp. He received the B. vol. I . . vol. Sonics Ultrasonics. pp.R. A. “Ferroelectric composites for hydrophones. 22. Berlincourt. Hisresearchinterests are in the fieldof dielectricand piezoelectriccrystals. A . pp. P. R . 1961. [31] B. R. H. vol.S.Tech.“Dynamicbehavior of periodic piezoelectric composites.degree in 1965 andtheM. he held positions with Leeds University as Lecturer (1948-1951) and as a research associate (1954-1961). [l61 G. 1954.’’ D?namic Response of Composite Materials.” IEEE Trans. SonicsUltrason. Ward. Sonics Ultrason. England. Kosoff. M.Ed. pp. Newnham. A. pyroelectricandelectrostrictivephenomena. Soc.E. vol.” Ferroelectrics. ceramic preparation.38. “The effects of backings and matching on the performance of piezoelectric ceramic transducers.. 2. and W.” Mater. 1975. vol. Newnham. NY. electrostriction and phase transitions. 2. E n g . phase transitions in ferroic materials.” Proc.” Ferroelectrics.Shrout. pp. 1977. in Bangalore. Amust. : PIEZOELECTRICCOMPOSITEMATERIALS-PART I [ S ] R.” in Physrcal Acoustics. Amer. 1981. H. (“84) was born on December 8. R . degree in solid state science from The PennsylvaniaStateUniversity. Bowen. [23] T. and L. in 1961. E. Safari. vol.from The Pennsylvania State University.Schulze. “Piezoelectric 3-3 composites..D. (Fall meeting of the Society for Experimental Stress Analysis). D. SU-26. Christopher. electronic ceramics and their applications. “The design of efficient broadband piezoelectric transducers. [30] R . 1161-1169.degrees in solidstate science in 1968 and1973.is Fellow ofMineralogical the Society of America. Davidson.” IEEE Trans. 1-19.” in Proc.piezoelectricandpyroelectriccrystals. and R .” Phys. Sonics Ultruson. SonicsUlrrason. A. R .Sc. Desbois. ViscoelasticProperties of Polymers. E. BiomedicalUltrasonics. Shrout. 1979.degree in crystallography from Cambridge University. Goll and B.. R. R. HeobtainedtheB. 75-81.degrees in physics fromLeeds University in 1948 and1952. Gururaja was born on September 24. 7-14. J. Phys. SU16.193-200.S. Desilets. pp.India. Oneonta. 1984. Jaffe. Lees. Mason. 1979. E.andPh. in Leeds. Wang.. piezoelectric.Tancrell. Defranould. E. 3. Mason. [28] D. [l81 J. E. pp.H.. “High-frequency applications of PZT-polymer composite materials.[ 101 G . Gururaja. Chap. pp. in 1950 and theM.” Ferroelecfrics.respectively. 189-195. Holland. [20] S.Sc. vol. he worked as Research Associate and Assistant Professor i n the Massachusetts Institute of Technology. Jr. 161 K. C . 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. respectively. Klicker.Sc. in 1960.Cross. 1983. vol. and W.” Ferroelecrrics. Erikson. M. Wells. T. 1271W. pp. 1245-1248. L. [25] J.Arditi. vol. “Continuous poling of PZT fibers and ribbons and its application to new devices. Symp. 1943.Guraraja. [8] H . 1923. Cross. 1596-1608.A.pp. 1980. “Tone-burst testing of pulse-echo transducer.Cross.pp.S.’’ Ferroelectrics.70. SU-13. and W.Schulze.pp. Schulze. England. Walter A. Blomed. W. BME30. respectively. pp. vol.Rittenmyer.” submitted to IEEE Trans. 1982. [l91 J. Sessler. NY. R. Callerame.41. S. New York: John Wiley. Sonics U/rrasonics.and S.D. 1980. Suppl. Appl. Currently.

SU-32. AND VOL.498 IEEE TRANSACTIONS ON SONICS ULTRASONICS. JULY 1985 . 4. NO.