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Received 2 March 2015; Revised 4 May 2015; Accepted 7 May 2015; Published 19 June 2015
Piezoelectric materials have been vastly used in ultrasonic transducers for medical imaging. In this paper, firstly, the most promising
lead-free compositions with perovskite structure for medical imaging applications have been reviewed. The electromechanical
properties of various lead-free ceramics, composites, and single crystals based on barium titanate, bismuth sodium titanate,
potassium sodium niobate, and lithium niobate are presented. Then, fundamental principles and design considerations of ultrasonic
transducers are briefly described. Finally, recent developments in lead-free ultrasonic probes are discussed and their acoustic
performance is compared to lead-based transducers. Focused transducers with different beam focusing methods such as lens
focusing and mechanical shaping are explained. Additionally, acoustic characteristics of lead-free probes including the pulse-echo
results as well as their imaging capabilities for various applications such as phantom imaging, in vitro intravascular ultrasound
imaging of swine aorta, and in vivo or ex vivo imaging of human eyes and skin are reviewed.
Keywords: Lead-free; piezoelectric; ultrasonic transducers; medical imaging.
1. Introduction
Piezoelectric materials generate polarization under application of a mechanical force. The generated polarization is
proportional to the applied force via a proportionality coefficient which is called the piezoelectric constant (dij ). Piezoelectric materials also exhibit a reverse piezoelectric effect
which is an electric field-induced displacement. The mechanical strain generated in these materials is also proportional to the applied electric field through the piezoelectric
constant.15
Ferroelectric materials are a subcategory of piezoelectrics
in which the direction of polarization can be switched by
application of an external electric field. Due to the internal
friction required to nucleate and switch ferroelectric domains
in different crystallographic orientation, ferroelectrics have a
characteristic hysteresis loop with a coercive field (the electric field required to switch the domains) and a remnant polarization. The remnant polarization in ferroelectrics is
permanent and does not disappear upon removing the electric
field. This is opposite to nonferroelectric piezoelectrics such
as ZnO, AlN, and quartz as well as anti-ferroelectrics which
do not possess a remnant polarization after the electric field is
removed.1,2,48
Due to their special characteristics, piezoelectric materials
have found hundreds of civil, military, and energy-related
applications. Automotive, computer, medical, and electronic
industries are the main customers of piezoelectric materials.
Disposable patient monitors, heart monitors, catheters, and
This is an Open Access article published by World Scientific Publishing Company. It is distributed under the terms of the Creative Commons Attribution 3.0
(CC-BY) License. Further distribution of this work is permitted, provided the original work is properly cited.
1530002-1
Moderate
Severe
Lethargy
Anorexia
Abdominal discomfort
Arthralgia
Anemia
Headache
Abdominal cramps
Gingival lead line
Peripheral neuropathy
Convulsions
Coma
Encephalopathy
Renal failure
lead-free piezoelectrics. This ceramic also showed a remarkable clamped dielectric constant " S33 ="0 of about
2820. However, the low Curie temperature of BZT50BCT
ceramic (TC 93 C) restricts the application of this lead-free
piezoelectric ceramic.23,24
1.2. BNT-based ceramics
1530002-2
1000
490
730
440
1160
Td ( C)
d33
(pC N 1 )
k33 (%)
Ref.
113
185
150
220
170
181
92
125
84
174
56
48
55
47
61
34
34
30
31, 34, 36
31, 34, 36
TC
( C)
d33
TtO
( C) (pC N 1 ) kp (%)
KNNBKT
1260
376
75
KNNLT
5401256
323
70
KNNLS
1380
368
35
KNNLTLS
6651865 265290 60
Ba-doped
1173
266
70
KNNLTLS
CuO-doped
1230
264
40
KNNLTLS
251
200230
265
315
210
260
56
3651 41, 51
50
46, 52
48.4 57, 58
34.8
57
48
59
Besides piezoelectric ceramics and single crystals, piezoelectric/epoxy composites have also been used as the active
layer in ultrasonic transducers particularly in high frequency
probes for medical imaging. These composites offer several
advantages in comparison to monolithic piezoelectric ceramics or polymers. High coupling coefficient, low acoustic
impedance, better acoustic matching to the human body,
adjustable dielectric constant, and mechanical flexibility are
some of the benefits of piezoelectric composites.62 Composite materials show higher g33 coefficient (g33 d33 =" T33 )
than ceramics which results in a better sensitivity in the receiver mode.
Dice-and-fill method is a traditional technique for fabrication of 13 composites.60,62 Injection molding, lost mold,
tape lamination, relic processing, laser ultrasonic cutting, jet
machining, 3D printing and reticulation are some of the other
techniques used for fabrication of piezoelectric composite
with various structures.6466 Figure 1 illustrates a modified
dice-and-fill method to prepare 13 piezoelectric/epoxy
composites. Table 4 provides properties of several lead-free
composites used in fabrication of ultrasonic transducers.
1.6. Ultrasonic transducers
Ultrasonic transducers are composed of three main components: a piezoelectric material, a backing material and one or
Fig. 1. Schematic illustration of the modified dice-and-fill method used for fabrication of 13 composites.60
1530002-3
KNNLT composite
BNTBT composite
BNTBT fiber
composite
d33 (pC/N)
kt
Z (MRayl)
Ref.
140
360
72
300
600
588
0.65
0.73
0.71
6.6
16
61
60
62
fH fL
100;
fc
Eq. (3)36,7173:
p
Zwater ZCeramic ;
q
3
2
Zceramic :
ZM Z water
ZM
2
3
a2
f
a2 c ;
C
where a is the radius of the transducer, C is the sound velocity, and is the wavelength corresponding to the transducer center frequency ( fc ).
The lateral (Rlat ) and axial (Rax ) resolutions of the transducer can be calculated from Eqs. (7) and (8), respectively36:
F
;
2a
C
Rax
;
2f
Rlat
7
8
where the F is the focal length, 2a is the diameter of transducer, C is the sound velocity and f is the frequency width
( fhigh flow ).
Lens-focusing is the most common method to focus the
ultrasound beam and improve the resolution. Usually convex
lenses made of elastomers such as room temperature vulcanization (RTV) and Sylgard silicone with a sound velocity
less than the speed of sound in water ( 1480 m/s) are bonded
on top of outer matching layer. The focal length (F) of the
lens-focused transducers can be calculated by the following
equation76:
C 1
F R 1 2
;
9
C1
1530002-4
1530002-5
Normalized Amplitude
1.5
EXP
KLM
1
0.5
0
-0.5
-1
13.0
13.5
14.0
14.5
15.0
Time (s)
(a)
5
EXP
Magnitude (dB)
(a)
KLM
-5
-10
-15
-20
-25
-30
5
10
15
20
25
30
35
40
Frequency (MHz)
(b)
Fig. 5. (a) Pulse-echo waveform and (b) frequency spectrum of the
BSZT transducer.22
the transducer. This composition exhibited a thickness coupling coefficient (kt ) of 0.45 and clamped dielectric constant
of 350. Low dielectric constant is desired in single element
high frequency transducers for a better electrical matching
and improved lateral resolution (due to the larger aperture). In
addition, BNKLT88 ceramics possess a higher depolarization
temperature compared to other BNT-based compositions.36
The ceramic with thickness of 109 m was sandwiched between epoxy-tungsten backing and silver epoxy matching
layers to fabricate a single element transducer. The thickness
of backing layer was 1.3 mm to provide 30 dB round trip
acoustic attenuation around 20 MHz. The matching layer
thickness was determined based on the quarter wavelength
design rule. A curved Epotek epoxy lens was casted on the
matching layer to improve the acoustic performance.36
Figure 6 shows the pulse-echo waveform and frequency
spectrum of the focused transducer. The center frequency and
6 dB bandwidth were measured to be about 23 MHz and
55%, respectively.
Figure 7 illustrates an ultrasound image of a phantom
made of copper wires (30 m in diameter) acquired by a
BNT-based transducer. The results indicated that this
(b)
Fig. 6. Simulated (KLM model) and measured (a) pulse echo
responses and (b) frequency domains of a BNT-based lens-focused
transducer.36
1530002-6
d33 (pC/N)
kt
Qm
V(m/s)
Z(MRayl)
BNTBT single
crystal
BNTBT/epoxy
13 composite
430
1000
0.63
60
4800
29
360
600
0.73
4100
16
backing layer and the array kerf (70 m width) was filled
with an attenuative epoxy. The 6 dB bandwidth of both
single element and linear array transducers exceeded 100%.60
In order to image fine tissues for applications such as
ophthalmology and dermatology, high frequency transducers
with enhanced resolution are required.62 Traditional diceand-fill method has limitation for fabrication of composites
with very fine elements and small pitches. Fiberepoxy
composites can be regarded as an alternative method for
preparation of high frequency transducers.62 Using solgel
method, Wang et al. prepared BNTBT fibers with diameter
of about 150 m.62 13 composites were processed by
aligning fibers in a plastic tube followed by epoxy filling
(Fig. 9).
The ceramic volume fraction and thickness of the composite were 30% and 143 m, respectively. The thickness
coupling coefficient kt of the composites was 0.71 which
was considerably greater than that of monolithic ceramic
(kt 0:45). A 14 MHz focused transducer was fabricated by
forming a convex shape on the composite attached to silicone rubber as the backing material. The 6 dB bandwidth
and IL of the transducer were measured to be 80% and
34.8 dB.62
2.3. KNN-based transducers
KNN-based transducers for medical imaging application
were developed by Jadidian et al.55 The acoustic performance of a 25 MHz single element transducer with
(K0:44 Na0:52 Li0:04 )(Nb0:84 Ta0:10 Sb0:06 )O3 (abbreviated to
KNNLTLS) active element was compared to a PZT
fiber 13 composite transducer. The properties of KNNbased ceramics and 13 PZT composite are given in
Table 6. The KNNLTLS transducer exhibited a 6 dB
bandwidth of 70% and IL of 21 dB. The electrical impedance of KNN-based piezoceramic was close to 50 ,
1530002-7
d33 (pC/N)
tan
kt
KNNLTLS
13 PZT fiber composite
175
400
644
541
506
296
0.022
0.013
0.39
0.64
(a)
(b)
(c)
(d)
Fig. 10. The time and frequency domain spectra of (a)-(b) the 13 PZT fiber/polymer composite and (c)-(d) KNNLSLT transducer.55
1530002-8
Piezoceramic
First matching
silver epoxy
Second matching
silver epoxy
Backing material
Za
ta
Zm1
tm1
Zm2
tm2
Zb
tb
31
75
7.3
8.4
2.5
13.0
5.9
> 3 mm
(a)
Material
Dimpled KNNBKT
ceramic
Dimpled PMN0.28PT
single crystal
Plane PMN0.28PT
ceramic
Fc
(MHz)
6 dB
BW%
IL
(dB)
Axial
resolution
(m)
Lateral
resolution
(m)
40
72
28.8
44
125
34
75
22.9
58
131
29
30
21.8
(b)
Fig. 12. In vitro imaging of swine aorta acquired by (a) a dimpled
PMNPT and (b) a dimpled KNN-based probes.82
1530002-9
(a)
(b)
(a)
Fig. 14. High resolution in-vivo images of (a) a nail finger and
(b) naevus of human forearm skin.
(b)
Fig. 13. In vivo images of a naevus of human forearm acquired by
(a) a 30 MHz lead-free probe and (b) a 20 MHz PZT-based probe.83
Material
Table 9. Physical and electromechanical properties of a KNN-based thick
films prepared by pad-printing method.
Material
KNN-based film
3140
31.4
90
34
11.3
LiNbO3 crystal
13 PZT Fiber
composite
PVDF
PbTiO3 ceramic
1530002-10
Thickness
(m)
Zbacking
(MRayl)
Zmatching
(MRayl)
Focusing
technique
60
32
5.9
1
7.3
3
9
32
3.15
5.9
No
3
Spherical shaping
Spherical shaping
Material
Fc (MHz)
BW (%)
IL (dB)
Pulse
length (ns)
44.5
53.6
48.1
45.1
74
47
118
47
21.3
34.4
45.6
23.7
56
67
44
74
LiNbO3 crystal
13 PZT Fiber composite
PVDF
PbTiO3 ceramic
Fc (MHz)
Focusing
technique
Aperture
size (mm)
6 dB
BW (%)
IL
(dB)
Pulse
length (ns)
22
23
45
50
73
78
Lens
Spherical shaping
Lens
Spherical shaping
Lens
Spherical shaping
10
12
3.0
6.0
1.8
3.0
72
60
74
60
57
73
19.5
13.4
21.3
9.6
20.3
13.5
145
140
56
54
40
36
(a)
(b)
Fig. 15. (a) An UBM image of the anterior portion of an excised
human eye acquired by 40 MHz LiNbO3 transducer. (b) A wideangle view of a normal anterior human eye segment taken in vivo by
a 50 MHz transducer.87
1530002-11
(a)
(b)
Fig. 16. (a) Pulse-echo waveform and (b) frequency spectrum for LiNbO3 half-thickness inversion layer transducer.88
(a)
(b)
Fig. 17. Images of the posterior segment of an excised pig eye (a) fundamental imaging using the single element transducer and (b) harmonic
imaging using the dual element transducer.92
3. Conclusions
In this paper, the current state of lead-free ultrasonic transducers for medical imaging applications was reviewed.
Electromechanical properties of lead-free ceramics, single
crystals, and composites were summarized and promising
candidates with enhanced properties were identified. The
characteristics of the most encouraging lead-free transducers
along with the properties of their piezoelectric layer are
provided in Table 13.
Lead-free piezoelectrics have been successfully used in
fabrication of single element transducers, linear arrays, dual
frequency annular arrays, and inversion-layer transducers.
LiNbO3 single crystals are suitable for fabrication of single
element transducers with a large aperture. Depending on their
dielectric and electromechanical properties, BNT and KNNbased ceramics and single crystals could be utilized in single
element or array transducers. Transducers with wide range of
frequencies (3 to 80 MHz) for variety of imaging applications
Material
d33
" S33 ="0 (pC/N)
BSZT
1346
BZTBCT
2817
39
LiNbO3 crystal
KNNLTLS
506
(1173)
Ba 2 doped
KNNLTLS
KNNLT
890
BNTBT crystal
80
BNTBKTBLT
353
KNNBKT
730
PMN0.33PT
797
(Pb-based)
PbTiO3 (Pb-based) 200
1530002-12
kt
Fc
6 dB
(MHz) BW (%)
IL
(dB)
26
19
21
21
Ref.
300
597
35
175
210
0.45
0.41
0.49
0.39
0.37
42
30
45
26
5.5
76
53
54
72
50.5
22
22, 24
87
55
96
245
210
84
189
1430
0.42
0.52
0.45
0.50
0.58
40
25
22
40
44
45
46
61
72
45
18
32
28.6
28.8
15
79
78
36
82
97
50
0.49
45
47
24
86
Acknowledgments
The authors would like to appreciate the financial support of
Glenn Howatt foundation for continuous support of research
on lead-free piezoelectrics.
References
18
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74
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