3)O3-0.09PbTiO3 single crystals by domain observation

Accepted Manuscript Irreversible phase transition characteristic of 0.91Pb(Zn1/3Nb2/3)O3-0.09PbTiO3 single crystals by domain observation Rongfeng Zhu, Qihui Zhang, Bijun Fang, Jianning Ding, Xiangyong Zhao, Haosu Luo PII:

S1567-1739(16)30242-5

DOI:

10.1016/j.cap.2016.09.005

Reference:

CAP 4321

To appear in:

Current Applied Physics

Received Date: 4 August 2016 Accepted Date: 5 September 2016

Please cite this article as: R. Zhu, Q. Zhang, B. Fang, J. Ding, X. Zhao, H. Luo, Irreversible phase transition characteristic of 0.91Pb(Zn1/3Nb2/3)O3-0.09PbTiO3 single crystals by domain observation, Current Applied Physics (2016), doi: 10.1016/j.cap.2016.09.005. This is a PDF file of an unedited manuscript that has been accepted for publication. As a service to our customers we are providing this early version of the manuscript. The manuscript will undergo copyediting, typesetting, and review of the resulting proof before it is published in its final form. Please note that during the production process errors may be discovered which could affect the content, and all legal disclaimers that apply to the journal pertain.

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Irreversible phase transition characteristic of 0.91Pb(Zn1/3Nb2/3)O3-0.09PbTiO3 single crystals by domain

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observation

Rongfeng Zhu1, Qihui Zhang1, Bijun Fang*,1, Jianning Ding*,1,2, Xiangyong Zhao3, Haosu Luo*,3

School of Materials Science and Engineering, Jiangsu Collaborative Innovation

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1

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Center of Photovolatic Science and Engineering, Changzhou University, Changzhou 213164, China 2

School of Material Science and Engineering, Jiangsu University, Zhenjiang 212013,

China

Key Laboratory of Inorganic Function Material and Device, Chinese Academy of

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3

Sciences, Shanghai 201800, P. R. China *

Corresponding authors:

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E-mail addresses: [email protected] (B. Fang); [email protected] (J. Ding);

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[email protected] (H. Luo)

Tel.: +86 519 86330095; fax: +86 519 86330095

Abstract: In situ temperature dependent ferroelectric domains dynamic evolution of the (001)pc oriented 0.91Pb(Zn1/3Nb2/3)O3-0.09PbTiO3 (PZNT91/9) single crystals was observed by polarized light microscopy (PLM) and real time synchrotron-radiation (SR) X-ray white-beam topography. Intricate domain structures including monoclinic

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ACCEPTED MANUSCRIPT phase are distinguished by PLM at room temperature, and irreversible domain configuration dynamic evolution upon thermal cycling is observed by both methods. Such irreversible domain evolution combined with coexistence of multi-ferroelectric

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phases and polarization rotation may be related to the extraordinary piezoelectric performance in the ferroelectric single crystals with the morphotropic phase boundary (MPB) compositions.

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synchrotron radiation; white-beam topography

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Keywords: PZNT single crystals; ferroelectric domain; polarized light microscopy;

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ACCEPTED MANUSCRIPT 1. Introduction Since

the

development

of

the

relaxor-based

single

crystals

Pb(Mg1/3Nb2/3)O3-PbTiO3 (PMN-PT) and Pb(Zn1/3Nb2/3)O3-PbTiO3 (PZN-PT) [1-3],

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the mechanisms of the engendering of high piezoelectric response have gained great research interest, especially with the compositions around morphotropic phase boundary (MPB). Among various mechanisms, engineered domain configuration,

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polarization rotation theory, and symmetry-adaptive intermediate ferroelectric phase

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with low symmetry provide significant guidances for interpreting the origins of the extraordinary piezoelectric behaviors [4-8].

Due to the non-centrosymmetric crystal structure nature, complicate and versatile multiple domain structures tend to form in ferroelectric crystals to minimize Gibbs

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free energy, including local energy minimum and unique global minimum [9]. Such intricate domain configuration is composed of domains with different well-defined orientations, and is affected greatly by compositions and external loadings [10],

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therefore, systematic researches are essential to understand the relationships between

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domain structures, polarization rotation and piezoelectric performance. Optical observation method provides efficient way to detect symmetry of

ferroelectric crystals, in which the ferroelectric phase can be determined based on optical extinction law and allowable structures of domain walls [11]. By using optical polarized light microscope (PLM), monoclinic and orthorhombic ferroelectric phases were observed in many ferroelectric single crystals with the MPB compositions [10-14]. Such complex domain structures create intricate nonlinear local domain

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ACCEPTED MANUSCRIPT network, which reduces electrostatic energy and influences overall material performance. Synchrotron-radiation (SR) X-ray white-beam topography offers another convenient method to map dynamic domain behavior in real time due to its

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extremely strong intensity and natural high collimation [15,16]. Although encouraging advances were obtained on the piezoelectric response mechanisms, the understanding of the relationships between structure, domain

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configuration and piezoelectric performance was still a challenging work, especially

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the domain structure evolution under external loadings. Domain configuration was conceived formed accompanied by the notable ferroelectric phase transition (FPT), which exerted greatly effects on the anisotropic performance of ferroelectric materials [10]. Therefore, the dynamic behavior of domain configuration of the (001)pc oriented (PZNT91/9)

single

crystals

under

external

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0.91Pb(Zn1/3Nb2/3)O3-0.09PbTiO3

environmental temperature was studied by optical polarized microscope and SR X-ray white-beam topography in this paper, and an irreversible domain evolution was

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observed. Such study would be helpful for the designing domain configuration and

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tailoring physical performance of ferroelectric single crystals.

2. Experimental procedures The PZNT91/9 single crystals used in this experimental were grown by a

modified Bridgman method using an allomeric 0.69Pb(Mg1/3Nb2/3)O3-0.31PbTiO3 seed single crystals [17]. For domain observation, the crystal plates were cut perpendicular to the pseudo-cubic (001)pc orientation and polished to around 50 µm.

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ACCEPTED MANUSCRIPT Surface flatness of the polished PZNT91/9 crystal plates were measured by a di NanoMan VS atomic force microscope (AFM, Bruker Corporation) by means of PeakForce Tapping. Room-temperature domain configuration and optical extinction

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characteristic were observed by a Olympus BX51-P polarizing microscope (Olympus America Inc.). The domain structure evolution was observed in situ by a Nikon Eclipse 50iPOL polarizing microscope (Nikon Corporation), in which a Linkam

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THMS600 heating/cooling stage (Linkam Scientific Instruments) was attached to

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provide precise 1 °C/min heating and cooling processes [18], and by a SR X-ray white-beam topography in transmission mode (Beijing Synchrotron Radiation Laboratory) [15].

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3. Results and discussion

Fig. 1 shows typical AFM surface morphology of the (001)pc PZNT91/9 single crystals. The regular stripes maybe correlated with the ferroelectric domain

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configuration, which can be observed by AFM in piezoresponse force microscopy

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imaging technique from micro- to nano-meter scale [19]. 3-D surface topography reveals rather less corrugation of the surface, indicating that the mechanical polished crystal plates are rather smoothness, which are suitable for observation domain structures by optical method. Since the physical performance symmetry was included in the point group symmetry elements for crystals, the ferroelectric phase symmetry could be determined by analyzing the orientations of spontaneous polarization using the optical polarized

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ACCEPTED MANUSCRIPT microscope according to the crystallographic symmetry and optical extinction law [10]. Fig. 2 shows room-temperature domain configuration of the (001)pc PZNT91/9 plane crystal observed by Olympus PLM under unipolar polarized light and by Nikon

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PLM under crossed polarized light. Since the composition of the PZNT91/9 single crystals approaches to the notable MPB composition, complex domain structures composed of regular stripes and irregular shapes form when the crystals are cooled to

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below the Curie temperature, which can be attributed to the tetragonal ferroelectric

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phase and rhombohedral one due to their extinction angles being 90°, and 71° or 109°, respectively [14]. The color differences can be attributed mainly to the different polarized light method used.

Since the discovery of monoclinic and/or orthorhombic ferroelectric phase in

detect

such

low

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Pb(Zr1-xTix)O3 and related materials [7,8], PLM provides an efficient technique to symmetry

ferroelectric

phase

[10-14],

therefore,

the

room-temperature domain structures of the (001)pc PZNT91/9 plane crystal were

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observed further by Nikon PLM within the heating/cooling stage, which was used to

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observe the domain dynamic behavior under thermal cycling. Using the symbol P/A proposed by Hao Deng et al., i.e. the angle between the polarizer/analyzer and the reference direction, the extinction angles and therefore their crystal systems can be determined [14]. The plane crystal was rotate in-situ with an interval of 10° to find extinction phenomena, and typical domain images are shown in Fig. 3 as examples. To determine the crystal systems, the exact extinction angles were obtained by fine rotation around the extinction locations. In area 1, extinction occurs when P/A=θ=90°

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ACCEPTED MANUSCRIPT (the extinction angle), indicating that such area exists in tetragonal ferroelectric phase. Extinction is visible at θ=71° for area 2, proving that such region belongs to rhombohedra ferroelectric phase. As for area 3, non simple extinction angles appear,

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accompanied by large quantities of fine lamella domain walls. The extinction angle is between 30-40°, and does not appear repeatedly within the 180° rotation. Such extinction angle is permissible only in monoclinic ferroelectric phase. Based on the

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discussion of the optically biaxial M phases, area 3 belongs to monoclinic MA or MB

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ferroelectric phase [10,14].

Fig. 4 shows the domain configuration evolution upon heating of the (001)pc PZNT91/9 plane crystal. Also complicated domain structures are observed in the limited area, and more intricate successive domain changes are induced by heating.

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Using the circle labeled stripe as an example, complicated MPB and monoclinic domain configurations are determined at room temperature based on crystallographic symmetry and optical extinction law but with much difficulty [10-14]. When

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increasing to 85°C, miniature periodic lamellas are induced with different extinction

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color, confirming the different domain crystallographic symmetry along the labeled stripe. Further increasing to 140°C, twin-like domain zones, i.e., one of miniature lamellas and another of almost complete extinction dark, prove further the coexistence of complicate domain configurations. When the heating/cooling stage is above 200°C, the observed area becomes complete dark due to the complete extinction of the (001)pc PZNT91/9 plane crystal in the paraelectric state under the crossed polarized light.

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ACCEPTED MANUSCRIPT Since the determine of the successive ferroelectric phase transitions (FPTs) by optical observations is also difficult, other assistant methods are recommended to characterize the FPTs characters as our previous work did, in which the electric-field

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induced complex FPTs and their transition temperatures, i.e., the ferroelectric rhombohedral phase to ferroelectric monoclinic phase (FER-FEM), the ferroelectric monoclinic phase to ferroelectric tetragonal phase (FEM-FET) and the ferroelectric

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tetragonal phase to paraelectric cubic phase (FET-PC) transitions are detected clearly

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by the dielectric constant (ε), converse piezoelectric constant (d33), unipolar strain (S), and longitudinal electrostrictive coefficient (Q) dependency on temperature relationships

for

the

poled

0.35Pb(In1/2Nb1/2)O3-0.35Pb(Mg1/3Nb2/3)O3-0.30PbTiO3-Mn

Mn-doped (PIMNT-Mn)

single

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crystals [20]. However, due to the large residual elastic stain and space-charge field, such successive PFTs can not be induced only by poling for the PZNT91/9 single crystals [17]. Therefore, the detection of the low symmetry ferroelectric phases

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[21].

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requires other novel experimental methods or collective post treatments of materials

Fig. 4d shows the domain image of the (001)pc PZNT91/9 plane crystal cooling

to 140°C after the crystal was heated to 250°C and maintained for 5 min before cooling process. Needle stripes composed of 90° included angle cover across the wholly observed area, and no extinction occurs within the rotation of 360°. Such irreversible phenomena are reported for the first time, which indicates that the FTPs of the PZNT91/9 single crystals is irreversible based on the views of domain

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ACCEPTED MANUSCRIPT configuration evolution. After cooling to room temperature, the original domain structures can not be recovered and almost no macro domains are observed. Carefully slow cooling after heat treatment at far above the Curie temperature also can not

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recover the original domain configuration, which is usually effective in the PMN-PT single crystals and may be correlated with the large residual elastic strain energy due to lattice distortion and structure mismatch induced by the ferroelectric phase

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transition occurred in the PZNT91/9 single crystals [10,11].

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The room-temperature domain configuration of the PZNT91/9 single crystals via thermal cycling is observed further by the SR X-ray white-beam topography due to its high resolution (Fig. 5). The Laue spot among the many reflection spots is a projection of the crystal plane along the SR diffracted beam onto the film [15],

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therefore, detailed domain structure can be mapped easily by this topography method. Apparently different domain mapping is caused by thermal cycling, in which the dense regular stripes in the cooling crystal can be attributed to the lattice distortion

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and structure mismatch induced by the residual FPT stress upon cooling [10,11].

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Although the irreversible evolution of domain configuration is reported for the first time, such phenomena can not be isolated cases. In the work reported by F. Fang et al., the domain evolution and polarization rotation under electric field of the PMN-32PT single crystals were studied [10]. Under cyclic and static electric field loadings, the PMN-32PT crystal plates were recovered to zero-field state many times, whereas, the obtained domain configurations were apparently different although the authors discussed mainly on the multi-coexistence of ferroelectric phases [10]. A similar

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ACCEPTED MANUSCRIPT irreversible rhombohedral (tetragonal) to intermediate phase/orthorhombic phase transition was reported in the (Na,K)(Nb,Sb)O3-LiTaO3-xBaZrO3 lead-free ceramics induced by poling, although which was studied by the high resolution synchrotron

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X-ray and dielectric performance [13]. Such irreversible domain configuration evolution and complicate coexistence of multi-ferroelectric phases are associated with the intrinsic nature of ferroelectrics, which influence polarization rotation path and

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contribute to the ultrahigh piezoelectric activity in ferroelectrics with the MPB

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compositions [12,22].

4. Conclusions

In this work, the domain configurations and their dynamic evolution upon

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thermal cycling of the (001)pc oriented PZNT91/9 single crystals were studied by PLM and SR X-ray white-beam topography. Complicate domain configurations composed of tetragonal, rhombohedral and monoclinic MA or MB symmetry phase are

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demonstrated in the PZNT91/9 single crystals with the notable morphotropic phase

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boundary (MPB) composition by PLM at room temperature. Successive temperature-induced ferroelectric phase transitions are observed by both methods, where the MPB and monoclinic domain configurations experience complicated progresses upon heating, and exhibit irreversible domain evolution upon thermal cycling. Although the irreversible domain evolution is reported for the first time, such phenomena can not be isolated cases and may contribute greatly to the ultrahigh piezoelectric response in the relaxor-based ferroelectric single crystals with the MPB

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ACCEPTED MANUSCRIPT compositions combined with coexistence of polymorphic ferroelectric phases and polarization rotation.

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Acknowledgements The authors thank the Natural Science Foundation of China (No. 51577015), the Major Projects of Natural Science Research in Jiangsu Province (No. 15KJA43002)

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and the Priority Academic Program Development of Jiangsu Higher Education

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EP

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Institutions for financial support.

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ACCEPTED MANUSCRIPT References [1] S.-E. Park, T. R. Shrout, Characteristics of relaxor-based piezoelectric single crystals for ultrasonic transducers, IEEE Transactions on Ultrasonics,

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Ferroelectrics, and Frequency Control 44(5) (1997) 1140-1147. [2] B. Fang, J. Li, H. Xu, H. Luo, Growth and pyroelectric properties of [001]-oriented (1-x)Pb(Zn1/3Nb2/3)O3-xPbTiO3 single crystals, Applied Physics

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[22] M. M. Rahman, N. Yasuda, Electric field-induced switching of nanometer-sized twin related domains in 0.91Pb(Zn1/3Nb2/3)O3-0.09PbTiO3 single crystal near a morphotropic phase boundary composition, Solid State Communications

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ACCEPTED MANUSCRIPT Captions of figures and tables Fig. 1.

Typical AFM images of the (001)pc PZNT91/9 plane crystal.

(a) surface topography and (b) surface undulation morphology.

Olympus PLM (a) and by Nikon PLM (b). Fig. 3.

(a)-(d) Domain structure observed by Nikon PLM within the heating/cooling

stage of the (001)pc PZNT91/9 plane crystal.

Domain configuration evolution upon heating of the (001)pc PZNT91/9 plane

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Fig. 4.

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Domain structure of the (001)pc PZNT91/9 plane crystal observed by

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Fig. 2.

crystal. (a) room temperature; (b) 85°C; (c) 140°C; (d) cooling to 140°C. Fig. 5.

Room-temperature domain structure of the (001)pc PZNT91/9 plane crystal

mapped by the SR X-ray white-beam topography. (a) before thermal cycling; (b)

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cooling to room temperature after soaking at 250 °C for 5 min.

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a

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Fig. 1.

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a

Fig. 2.

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Fig. 3.

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Fig. 4.

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a

Fig. 5.

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Highlights

Intricate domain structures including monoclinic phase of the (001)pc oriented

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PZNT91/9 single crystals are distinguished by PLM at room temperature. Successive temperature-induced ferroelectric phase transitions are observed by PLM and SR X-ray white-beam topography.

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Irreversible domain configuration dynamic evolution upon thermal cycling is reported

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for the first time.

Such irreversible domain evolution may contribute greatly to the ultrahigh piezoelectric response in the relaxor-based ferroelectric single crystals with the MPB

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compositions.