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Structural Description of the Macroscopic Piezo- and Ferroelectric Properties of Lead Zirconate
Titanate and structural contribution to the Ferroelectric Fatigue
J. Rouquette1, M. Hinterstein2, J. Haines1, J. Glaum2, M. Knapp3, J. Eckert3, M. Hoffman2 and P. Papet1*
1
ICGM, UMR CNRS 5253, Université de Montpellier, Montpellier, France, 34095
2
School of Materials Science and Engineering, University of New South Wales, NSW, Australia
3
Institut für Werkstoffwissenschaften, Technische Universität Dresden, Dresden, Germany
*e-mail: [email protected]
PbZr1-xTixO3 (PZT) is an important class of ferroelectrics materials with the ABO3 perovskite-type structure
due to their exceptional dielectric and piezoelectric properties. It is well known that PZT ceramics and thin
films are sensitive to the level of stress induced by both external elastic and electric fields which
fundamentally modifies their physical properties. The “in situ” structural description of the ferroelectric
properties as a function of the applied electric field E, i.e. switching of the spontaneous polarization PS with
an electric field, is a useful approach to study the relationship between the structure of materials and their
macroscopic properties [1]. To investigate the cycled poling process of PZT, we performed X-ray
measurements at the high resolution powder diffraction station of the materials science (MS) beamline at
the Swiss Light Source (SLS, Villigen, Switzerland) on PZT sample with composition close to the
Morphotropic Phase Boundary (MPB). A setup was used to average the effects of the preferred orientation
induced by the strong piezoelectric strain and solve in situ the crystal structure as a function of the applied
electric field. Fig. 1 shows example on the structural dependence of this PZT sample as a function of the
applied electric field. It gives the tetragonal-monoclinic phase ratio measured with an applied electric field.
Based on this microscopic description of the macroscopic ferroelectric and piezolectric properties of MPB
PZT, we also investigated ferroelectric fatigue (which is characterized by the loss of the switchable
remnant polarization and strain as a function of the number of switching cycles) in this material by
synchrotron X-ray diffraction. We showed the structural difference between a non fatigued and a fatigued
sample arises from i) a less effective field induced tetragonal-to-monoclinic transformation and ii) a
significantly less intense and more diffuse anomaly of Biso(Pb)m, which accounts for polarisation flipping.
Finally, the structural contribution to the fatigue of PZT ceramics corresponds to a reduction in the degree
of tetragonal-to-monoclinic transformation (decrease in the piezo/ferroelectric efficiency) [2].
Figure 1. Monoclinic-Tetragonal phase ratio (%) of
PZT sample as a function of the applied electric field.
1. Structural Description of the Macroscopic Piezo- and Ferroelectric Properties of PZT, M. Hinterstein, J. Rouquette, J. Haines,
P. Papet, M. Knapp, H. Fuess, Phys. Rev. Lett. 107, 077602 (2011)
2. Structural Contribution to the Ferroelectric Fatigue in PZT Ceramics, M. Hinterstein, J. Rouquette, J. Haines, P. Papet, J. Glaum,
M. Knapp, J. Eckert , M. Hoffman, Phys. Rev. B 90, 094113 (2014)
Curriculum Vitae
Prof. Philippe PAPET, University Montpellier, FRANCE
Philippe Papet, born in 1959 in Bellac (Haute Vienne), France. In 1984 he
obtained an Engineering diploma (Master degree in Ceramic Materials) from ENSCI,
Limoges, France. He obtained the doctorate in Ceramic Materials from Limoges
University, France, in 1988 where the subject was the studying, for mechanical
applications, of phase transitions in pentavalent doped zirconia ceramics versus the
dopant contents and the densification of these ceramics by solid state sintering to control
the microstructure.
After one year as post doctorate in the Materials Research Laboratory in Penn
State University (State College), USA, studying the grain size effects on the dielectric
properties in relaxors ceramics, he moved in 1990 to Saint Gobain Company in Ceramic
department (Paris, France), where he worked as a research engineer on piezoelectric
materials. After Three years in industry, he moved in 1992 for an assistant professor
position at the University of Montpellier 2. He has been working as full Professor of Solid
State Chemistry at the same University from 1999.
Philippe Papet is the Author of 96 papers published on international scientific
journals with peer review and 2 international patents.
His scientific interests concern:
-
the studying of crystal growth of piezoelectric single crystals belonging
to the alpha quartz family, by hydrothermal and fluxes methods,
-
the determination of pressure-temperature phase diagram in the
PbZrO3-PbTiO3 system, where he is using neutron and synchrotron
radiation as well as laboratory X-ray diffractometers,
-
the synthesis of piezoelectric thin films for surface acoustic waves
applications,
-
the electrical conductivity in complex materials by using the
impedance spectroscopy. He has developed specially adapted cells
working at very high temperature to measure refractory oxides
conductivities.
-
The study of silicide compounds for the thermoelectricity
In 2004, 2008 and 2012 he organized a 3 days international workshop EWPM
(European Workshop on Piezoelectric Materials) dedicated to the scientists community in
the field of piezoelectricity. He was the editor in Solid State Sciences of some EWPM
selected papers (Solid State Sciences).
He was in 2010-2014 the co-director of Polytech (Enginery School of the
university de Montpellier 2, 1000 students). His teaching activities include lectures on
“ceramics” as well as “coupling properties and energy conversion in materials” for Master
and Polytech students.
For five years he has been leading the research team C2M (15 full time
researchers and 12 post-doc and doctorate students) belonging to Institute Charles
Gerhard UMR 5253, Montpellier France.
List of selected publications of Philippe Papet:
1 Ali Al-Zein, G. Fraysse, Jérôme Rouquette, Ph Papet, J. Haines, B. Hehlen, C.
Levelut, G. Aquilanti and Y. Joly: Zr-shift at the origin of the exceptional piezoelectric
properties of
PbZr0.52Ti0.48O3, Physical Review B, 81(17) , 2010,
4110
2 Jérôme Rouquette, Julien Haines, Ali Al-Zein, Philippe Papet, Françoise Damay,
Julie
Bourgeois, Tahar Hammouda, Fabrice Doré, Antoine Maignan,
Maryvonne Hervieu and
Christine Martin: Pressure-Induced Structural Transition
in LuFe2O4, Towards a New Charge
Ordered State, Physical Review
Letters, 105(23) , 2010, 237203
3
Pascale Armand, Marion Beaurain, Benoit Rufflé, Bertrand Ménaert and Philippe
Papet
Temperature dependence of single-crystal elastic constants of flux-grown alphaGaPO4
Inorg. Chem., 2009, 48 (11), pp 4988–4996
4 J. Rouquette, J. Haines, G. Fraysse, Ali Al-Zein, V. Bornand, Ph. Papet, S. Hull
and F. A. Gorelli| High-Pressure Structural and Vibrational Study of PbZr0.40Ti0.60O3,
Inorg. Chem.,
47(21), 2008
5 G. Fraysse, J. Haines, V. Bornand, J. Rouquette, M. Pintard, Ph. Papet and S.
Hull; Low- symmetry phases at the tilt boundary of the Pb,,Zr1−xTixO3 solid solution,
Phys. Rev. B, 77, 2008, 064109
6 J. Rouquette, J. Haines, V. Bornand, Ph. Papet and J L. Sauvajol : Use of
Resonance Raman Spectroscopy to study the phase diagram of PbZr0.52Ti0.48O3,
Phys. Rev. B, 73(224118), 2006, 1-5
7 M. Beaurain, P. Armand and Ph. Papet : Synthesis and Characterization of alphaGaPO4
single crystals grown by the flux method, Journal of Crystal Growth,
294, 2006, 396-400
8 J. Rouquette, J. Haines, V. Bornand, M. Pintard and Ph. Papet : Pressure-induced
rotation of the spontaneous polarization in monoclinic and triclinic PZT, Phys. Rev.
B, 71, 024112, 2005,
1-10
9 Ph. Papet, J. Rouquette, V. Bornand, J. Haines, M. Pintard & P. Armand :
"Structural transitions versus pressure and temperature in the PZT phase diagram",
J. Electroceramics,
13, 311-314 (2004)
10 J. Rouquette, J. Haines, V. Bornand, Ph. Papet, L. Konczewicz, F.A. Gorelli & S.
Hull :
"Pressure-tuning of the morphotropic phase boundary in piezoelectric lead
zirconate titanate", Phys. Rev. B., 70 (1), 014108, 1-4 (2004)