Materials Science and Engineering A336 (2002) 124
/128

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Stress dependence of reversible and irreversible domain switching in

PZT during cyclic loading
Jose M. Calderon-Moreno a,*, Monica Popa b,1
a
Materials Department, Queen Mary and Westfield College, University of London, London E1 4NS, UK
b
Romanian Academy, Institute of Physical Chemistry, Bucharest 77208, 202 Splaiul Independentei, Romania

Received 3 August 2001; received in revised form 19 November 2001

Abstract

Stresses suffered by lead zirconate titanate (PZT) components in actuators are the origin of the gradual degradation of the
microstructure and piezoelectric capability that limits their lifetime. The stress
/strain behavior of a PZT ceramic has been studied in
compressive uniaxial cyclic loading using a constant loading rate, in order to determine the operating stresses that cause structural
damage associated to the exhaustion of twinning. Domain switching strain curves have been calculated considering that stress-
induced switching of 908 domains is the mechanism responsible of non-linear stress
/strain behavior. Each load
/unload cycle caused
a permanent strain in the PZT. Successive cycles produced incremental increases in stress-induced permanent strain, up to a
maximum value or ‘saturated cyclic permanent strain’, attributed to irreversible stress-induced domain switching. The dependence
of the saturated permanent strain with the maximum cyclic load showed a characteristic non-linear behavior, with a steep slope at a
stress level sI, that we called the ‘critical stress for irreversible domain switching’. Below sI, the majority of domain switching is
reversible. We have called sR to the stress at which the increase in reversible domain switching is more pronounced. At stresses
between sR and sI high reversible strains can be reached without resulting in permanent stress-induced depoling and thus without
the exhaustion of available twinning during subsequent load cycles. At maximum cyclic stresses higher than sI, irreversible domain
switching accounts for the majority of strain and increase rapidly toward values close to the maximum 908 domain switching strain
available. The number of cycles to failure also had a strong dependence with the maximum cyclic stress. Cyclic stresses above the
critical stress caused a rapid accumulation of permanent strains, so the saturated value is reached after a few cycles, resulting in early
catastrophic failure, because of the exhaustion of reversible domain switching. # 2002 Elsevier Science B.V. All rights reserved.

Keywords: Lead zirconate titanate (PZT); Piezoelectric; Stress
/strain behavior; Stress-induced domain switching; Irreversible or permanent damage;
Cyclic uniaxial compression

1. Introduction permanent deformation by the irreversible switching of

Because of its high piezoelectric coefficient, lead
zirconate titanate (PZT) is widely used in transducers
and actuators, where components are subjected cycli-
cally to high stresses and therefore can be easily
damaged. The mechanical stressing of PZT produces
* Corresponding author. Present address: Materials and Structures
Laboratory, Tokyo Institute of Technology, 4259 Nagatsuta, Midori,
Yokohama 226-8503, Japan
E-mail address: calderon1@rlem.titech.ac.jp (J.M. Calderon-
Moreno).
1
Present address: Materials and Structures Laboratory, Tokyo
Institute of Technology, 4259 Nagatsuta, Midori, Yokohama 226-
8503, Japan.
0921-5093/02/$ - see front matter # 2002 Elsevier Science B.V. All rights reserved.
PII: S 0 9 2 1 - 5 0 9 3 ( 0 1 ) 0 1 9 7 6 - 1
908 domains. This leads to highly anisotropic deforma-
tion behavior for poled materials [1,2]. The threshold
stresses required to produce this switching are relatively
small. Studies of stress related effects in the piezoelectric
capabilities of PLZT ceramics [3,4] have demonstrated
that the application of external compressive stress can
lead to the disappearance of the hysteresis loop char-
acteristic of the piezoelectric effect by complete inhibi-
tion of 908 domain movement. Therefore, stress
/strain
curves provide important information about the com-
plex constitutive non-linear behavior in piezoelectric
ceramics [5,6]. An excellent mean of assessing the
irreversible strain that builts up in a piezoelectric
material during operation is the study of its mechanical
response under cyclic stress [7]. Stress
/strain curves are
 J.M. Calderon-Moreno, M. Popa / Materials Science and Engineering A336 (2002) 124
/128
useful for the modeling of grains interaction and the
prediction of irreversible strains during operation that
are the origin of electromechanical fatigue. Simple
micro-mechanical models of stress-induced domain
switching can reproduce mechanical curves generated
in compressive tests in PZT materials [8], so that domain
switching coercive stresses and levels of internal stresses
associated to domain switching processes can be deter-
mined from the mechanical behavior. However, a
general micro-mechanical model for PZT ceramics able
to predict the microstructural evolution of piezoelectric
components during operation in actuators remains to be
developed. Accurate experimental characterization of
the mechanical response of piezoelectric materials is one
of the basis for understanding the constitutive laws of
electromechanical coupling, and therefore necessary to
develop more reliable micromechanical models able to
define operating conditions to increase the lifetime of
piezoelectric components. This research deals with the
formation of permanent stress-induced domain switch-
ing strain under cyclic loading at different levels of
maximum mechanical load.
2. Experimental
A commercial PZT-4 type material was used. Samples
used were cut from original plates into parallelepipeds
with dimensions 4 2 2 mm and well-aligned flat
surfaces prepared by sequential diamond polishing,
down to 1 mm. The specimens were poled before
mechanical testing.
The polarized samples were subjected to uniaxial
compressive stress parallel to the direction of polariza-
tion, along the longer axis of the specimen, and the
stress
/strain curve were measured. Compressive tests
were carried out in load control in an Instron type
apparatus at constant loading rate of 10 MPa s 1, up to
maximum loads of 600 MPa. Displacements/strains
were measured with a purposed built capacitance device
with a sensitivity of less than 1 mm. A detailed diagram
of the experimental device and compression jigs used
can be found elsewhere, along with details of specimen
preparation [7].
An illustration of the calculation method used to
obtain the ferroelastic contribution can be found in [9].
Strains associated to domain switching during mechan-
ical loading have been calculated by subtracting the
linear elastic contribution from the experimental stress
/
strain curve. Domain switching was considered the only
plastic deformation mechanism available. This ap-
proach is realistic in PZT, given the low level of stresses
necessary to activate the twinning of ferroelectric
domains, compared with any other deformation me-
chanism [5,6].
125
3. Results and discussion
3.1. Stress
/strain
Fig. 1 shows the evolution of stress-induced domain
switching strains during the first load-unload cycle. At
low stresses the behavior is almost linear, up to s1  100
MPa. At higher stresses (s2 400 MPa) domain switch-
ing has been exhausted and cannot be further increased.
When the sample is unloaded, some domains switch
back, but not all, because the strain does not decrease to
zero. After unload, relaxation of domains switching
back occurs for a period of several minutes until the
remaining strain in the unloaded sample reach a
permanent value. The permanent strains are produced
by domains that remain reoriented, producing depoling.
It is possible to fully reverse this permanent strain by
repoling if no microcracks had been created.
When a second loading cycle is performed, a similar
curve is obtained, and a second permanent strain is
added to the one created in the first cycle. Successive
cycles lead to the incremental accumulation of perma-
nent strain.
3.2. Permanent strain
Fig. 2 illustrates the incremental accumulation of
permanent strains observed after repeated cycles at
stress levels below the non-linear part of the domain
switching curve (s1) and above the non-linear part, once
domain switching has been exhausted on loading (s2) at
first cycle. In the latter case, the creation of permanent
strains is more severe at the early cycles, nearly
exhausting available domain switching after only four
Fig. 1. Stress-induced domain switching during the first load
/unload
cycle for the PZT material, calculated assuming that ferroelastic only
domain is responsible for the non-linear behavior. There is a
considerable relaxation after unload that results in a significant
reduction of the permanent domain switching below the first apparent
level observed at zero stress (marked by an arrow).
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Fig. 2. Evolution of permanent strains after cyclic loading with the
number of cycles, for a low stress level (s1) in the region showing
nearly linear stress-induced domain switching in Fig. 1, and for a high
stress level (s2), in the region where domain switching has been
exhausted in Fig. 1.
cycles. After repeated cyclic load, a saturation level of
permanent strain is achieved for any stress level, without
further increments occurring in new cycles.
Our previous research indicated that the permanent
strains generated in cyclic tests can be correlated to
electromechanical fatigue effects observed in piezoelec-
tric actuators [7] and that the extent of microcracking
created in the plastic deformation zone below the
indentor in indentation studies seemed to be inversely
related to the availability of twining modes in several
PZT materials [10,11]. The current research is aimed to
clarifying the evolution of the incremental accumulation
of permanent strains with cyclic loads and its effect in
the lifetime of the PZT during cyclic loading.
The saturated permanent strains are shown in Fig. 3,
compared with domain switching strain at first loading.
When compared with the stress-induced domain switch-
ing measured during the first load
/unload cycle, the
difference between the two curves can be related to the
remaining reversible domain switching available at that
stress. At 140 MPa the slope of the domain switching
strain versus stress curve is maximum and therefore
where the accumulation of domain switching strain is
more rapid. We have called sR the stress at which the
increase in reversible domain switching is more pro-
nounced. We will see later that it also corresponds to the
minimum coercive stress needed to initiate irreversible
domain switching. Below sR, the amount of irreversible
switching is significantly lower than that of reversible
switching. Above sR, irreversible switching occurs
rapidly. Irreversible domain switching given by the
saturated cyclic permanent strains curve already ac-
counts for the majority of domain switching strain at
210 MPa. Consequently, there is also a rapid
exhaustion in the reversible domain switching available
Fig. 3. Saturated permanent strains reached after cyclic loading at
different maximum loads in compression tests for PZT, compared with
the stress-induced domain switching measured during the first load
/
unload cycle. At sR ( 140 MPa) the slope of the domain switching vs.
stress curve is maximum and therefore the accumulation of domain
switching strain is more rapid. At sI (  230 MPa), the accumulation
of irreversible domain switching with stress is a maximum.
when we applied stresses higher than sR. The critical
value at which d(irreversible domain switching)/d(stress)
is maximum is shown in Fig. 3 as sI ( 230 MPa). We
have called sI the ‘stress for maximum irreversible
domain switching’ as opposed to sR at which the rapid
accumulation of strain corresponded mainly to rever-
sible domain switching.
Fig. 4 shows the evolution of reversible and irrever-
sible strain after saturation of permanent strains occurs,
in stable cyclic loading conditions. It can be noticed that
even at stress values over the initial coercive stress at
first cycle (50
/100 MPa) most of the domain switching
is reversible, but reversible domain switching decreases
rapidly for increasing stress levels. Just above sR, at
160 MPa, the ratio of reversible strain to irreversible
strain reaches a maximum. Reversible domain switching
accounts for about 70% of the maximum strain at that
stress. Above that stress any new strain created is
irreversible but also part of the reversible strain becomes
irreversible, so irreversible strain grows more rapidly
than the total strain at the expense of reversible domain
switching. At  210 MPa, just below sI ( 230) half of
the total strain is irreversible. The existence of reversible
domains implies the presence of twins that can be easily
switched in the case of stress concentrations during
grains interaction [3]. Therefore, operating conditions
that cause the exhaustion of reversible twinning have a
strong risk of causing rapid mechanical degradation by
microcracking in defect areas. Our investigation high-
lighted that that the presence of accommodating twins,
critical in the creation of microstructural damage, is still
significant at stresses (160
/210 MPa) much higher than
 J.M. Calderon-Moreno, M. Popa / Materials Science and Engineering A336 (2002) 124
/128 127

Fig. 4. Stress
/strain curves for reversible and permanent irreversible domain switching strain after cyclic loading in compression tests for PZT,
compared with the stress-induced domain switching available measured from the first load cycle. Critical or coercive stress for domain switching at
first cycle (sR) and for irreversible cyclic switching (sI) are indicated in the stress axis.

the coercive stresses for domain switching at first cycle

(50
/100 MPa). At stresses of 200 Mpa, more than 85%
of the twinning can be mechanically induced, but
reversible switching at this stress still accounts for above
half of the available domain switching strain at this
stress. On the other hand, for a stress of 300 MPa, the
total switching strain increase to almost 100%, but more
than 90% of it stay permanently switched after repeated
cycles. Therefore, the ability of the piezoelectric material
to accommodate local stresses is inhibited by the
application of high loads above a critical stress for
irreversible switching, with otherwise little gain on the
total switching strain. The lifetime of the material can be
seriously compromised if the piezoelectric displacement
of the actuator is used to a maximum, specially during
cyclic operation, because the exhaustion of reversible
switching will promote the creation of structural da- Fig. 5. Cycles to failure vs. maximum cyclic stress, at values of one to
four times the domain switching coercive stress in the first cycle (sR).
mage. For the hard piezoelectric studied here, almost The arrows at lower stresses means that no observed in Fig. 4 marks
90% of the maximum domain switching can be activated the transition between the regions of stable cyclic behavior and early
at a stress of 250 MPa; operation under higher stress will catastrophic failure. Stable cyclic behavior was observed at stresses
be almost meaningless in terms of piezoelectric actuator where reversible twinning is available, and can therefore act as a stress
relief mechanism.
displacement, but highly deleterious for the microstruc-
ture and the long term cyclic performance, as it was
confirmed by early failure. during cyclic loading is therefore highlighted. The
The number of cycles to failure was studied at present results indicate that the availability of reversible
different maximum stress levels (Fig. 5). At stresses domain switching in PZT during cyclic load hinders the
below the stress for maximum domain switching at first formation of irreversible structural damage at lower
cycle (sR  140 MPa) no early catastrophic failure was loads. On the other hand, after a few cycles at the higher
observed, and 50 load cycles were carried out without loads, the domains cannot switch-back during unload-
failure. Above the critical stress for maximum irrever- ing and no available twining modes remain. Once fully
sible domain switching ( 230 MPa) very rapid failure reversible switching is exhausted, there is no accommo-
occurred after a few cycles. At the highest loading, dation mechanism that can prevent the formation of
failure occurred already in the second loading cycle. The microcracks and structural damage in the weak inter-
importance of the exhaustion of irreversible switching faces of the PZT, a material characterized by high
128 J.M. Calderon-Moreno, M. Popa / Materials Science and Engineering A336 (2002) 124
/128
piezoelectric coefficient and very low fracture toughness
[2], and the lifetime of the material during cyclic load
decreases very rapidly.
The present work also points out to the effect of
mechanical load to prevent domain switching when
electric fields are applied in a PZT actuator component.
Given the limited strength of PZT, high electric fields
have to be avoided for a stable cyclic performance.
4. Summary
The behavior of a hard PZT under cyclic mechanical
loading has been investigated. The stress-induced do-
main switching behavior of our PZT revealed the
existence of saturated values of permanent cyclic strain
with a strong dependence of the maximum cyclic load.
Saturated permanent strains accounts for the smaller
part of the total domain switching strain available at
stress levels below a critical value called the ‘coercive
stress for irreversible domain switching’. That critical
stress is nearly two times (230 MPa compared with 140
MPa) the coercive stress for domain switching in the
first loading cycle. Results indicates that a stable cyclic
performance based on the switching of reversible
domain, without permanent degradation of the material,
can take place for levels of domain switching as high as
80% of the total at first cycle. However, permanent
strains increase very rapidly during cyclic loads over the
critical stress for irreversible switching. Operation at
stresses over the observed critical stress for irreversible
switching sI, at which domain switched become rapidly
exhausted, lead to rapid accumulation of structural
damage and catastrophic failure after a few loading
cycles. The results suggest that less than the maximum
domain switching and piezoelectric displacement should
be used during operation for a good cyclic performance
and lifetime of piezoelectric actuators, especially in PZT
components.
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