Available online at www.sciencedirect.com CERAMICS INTERNATIONAL Ceramics International 41 (2015) S458–S463 www.elsevier.com/locate/ceramint Comparison of structural, ferroelectric, and strain properties between A-site donor and acceptor doped Bi1/2(Na0.82K0.18)1/2TiO3 ceramics Thi Hinh Dinha, Mohammad Reza Bafandehb, Jin-Kyu Kanga, Chang-Hyo Hongc, Wook Joc, Jae-Shin Leea,n b a School of Materials Science and Engineering, University of Ulsan, Ulsan, Republic of Korea Department of Materials Science and Engineering, Faculty of Engineering, University of Kashan, Kashan, Islamic Republic of Iran c School of Materials Science and Engineering, Ulsan National Institute of Science and Technology, Ulsan, Republic of Korea Received 26 October 2014; accepted 14 March 2015 Available online 31 March 2015 Abstract Effects of Li- and La-doping on the structural, ferroelectric, and strain properties of Bi1/2(Na0.82K0.18)1/2TiO3 (BNKT) ceramics were compared. In this study, Li þ was selected as the A-site acceptor and La3 þ as the A-site donor. Li doping resulted in hardening of BNKT with an improved mechanical quality factor (Qm) of 253 and an increased coercive field (Ec), while La doping brought about a softening effect that was evidenced by an improved piezoelectric constant (d33) of 172 pC/N and decreased Ec. In addition, the large normalized bipolar strain (Smax/Emax) was obtained up to 650 pm/V in 3 mol% La-doped BNKT. & 2015 Elsevier Ltd and Techna Group S.r.l. All rights reserved. Keywords: B. Defects; C. Ferroelectric properties; C. Piezoelectric properties; Solid state reaction 1. Introduction Recently, lead-free piezoelectric ceramics have been extensively studied from both physical and technical points of view. Among various lead-free materials, binary (Bi,Na)TiO3–(Bi,K)TiO3 (BNKT) solid solutions are considered as potential candidates due to their excellent electromechanical properties near the morphotropic phase boundary (MPB) [1–4]. A number of previous studies have reported that electromechanical properties can be improved by modification of the MPB composition with various dopants or modifiers, such as BNKT–BiAlO3 [5], BNKT–LiSbO3 [6], Nb-doped BNKT [7], Ta-doped BNKT [8], Sn-doped BNKT [9,10], Li- and Ta-codoped BNKT [11], BNKT–LaFeO3 [12], Ladoped BNKT [13], and Ta-doped BNKT–LiSbO3 [14]. It has been well known in Pb-based piezoelectric ceramics that the hardening or softening through the addition of dopants n Correspondence to: University of Ulsan, P. O. Box 18, Nam-Ulsan, 680-749, Republic of Korea. Tel.: þ 82 52 259 2286; fax: þ82 52 259 1688. E-mail address: jslee@ulsan.ac.kr (J.-S. Lee). http://dx.doi.org/10.1016/j.ceramint.2015.03.150 0272-8842/& 2015 Elsevier Ltd and Techna Group S.r.l. All rights reserved. is a key technique to tailor their properties [15–17]. The best known examples are hard and soft Pb(Zr,Ti)O3 (PZT) ceramics, the most widely used piezoelectric materials. Hardening can be induced by the addition of acceptor dopants [18]. A better understanding of the hardening and softening in Pbbased ceramics has been presented by Chandrasekaran et al. [19]. Oxygen vacancies in acceptor (Fe) doped PbTiO3 (PT) are responsible for the formation of polar defect complexes. Both of the “bulk effects” and the “domain-wall effects” contribute similarly to the hardening phenomenon [19], while donor (Nb) doping increased domain mobilities, resulting from the lack of polar defect complexes. The effects of donor (Nb5 þ , Ta5 þ ) doping on the electromechanical properties of lead-free Bi0.5Na0.5TiO3 ceramics have been also reported [20]. In 2012, Han et al. [21] also compared the effects of Bsite acceptor and B-site donor doping and they found that donor-doping contributed to the destabilization of ferroelectric phases. More recently, the electromechanical properties of Mn- or Fe-doped BNT–BKT–Bi0.5Li0.5TiO3 piezoelectric ceramics were examined by Taghaddos et al. [22] in 2014. It T.H. Dinh et al. / Ceramics International 41 (2015) S458–S463 was found that the acceptor dopants can slightly decrease the optimum sintering temperature and enhance the mechanical quality factor considerably. Therefore, there is a great attraction from both scientific and technical points of view to investigate the effects of A-site acceptor as well as A-site donor on the piezoelectric properties of lead-free BNKT ceramics. In BNKT system (near MPB), due to difference between the ionic radius of doping elements and lattice ions, there are limited acceptor ions that can occupy the A-site ( e.g. Li þ , Rb þ , Cs þ ) or B-site ( e.g. Fe3 þ , Mn3 þ , Al3 þ ) and restricted donor ions that can substitute into A-site (e.g. In3 þ , Tl3 þ , La3 þ ) or B-site ( e.g. Ta5 þ , Nb5 þ , Sb5 þ ). This work compared the crystal structure, ferroelectric, and electromechanical properties of Li- and La-doped BNKT ceramics. It is expected to see a hardening effect in Li-doped BNKT ceramics due to creation of oxygen vacancies when Li þ ions occupy the A2 þ -sites. In contrast, a softening effect is presumed in La-doped BNKT ceramics due to generation of A-site vacancies when La3 þ ions substitute doubly charged A2 þ -site ions. The oxygen vacancies or A-site vacancies created in the lattice are compensated by the incorporated acceptor or donor ions, respectively. This can be understood by considering the Schottky defect reaction 0 LiA -LiA þ 1=2VO ð1Þ LaA -LaA þ 1=2V″A ð2Þ where VO and VA indicate oxygen and A-site vacancies, respectively. 2. Experiments Ceramic specimens with composition of [Bi1/2(Na0.82K0.18)1/ ] 2 1 xAxTiO3 (A ¼ Li or La; x ¼ 0.00–0.05), abbreviated as A100x, were synthesized using a conventional solid state reaction route. Reagent grade Bi2O3, Na2CO3, K2CO3, TiO2, Li2CO3, and La2O3 (99.9%, High Purity Chemicals, Japan) powders were used as raw materials. These reagents were dried S459 in an oven at 100 1C for 24 h and then weighed according to the formula. The powders were mixed in ethanol with zirconia balls by ball milling for 24 h, dried at 80 1C for 24 h, and calcined at 850 1C for 2 h in an alumina crucible. After calcination, the powder was mixed with polyvinyl alcohol as a binder and then pressed into green discs with a diameter of 12 mm under a uniaxial pressure of 98 MPa. Green pellets of Li100x and La100x were sintered at 1100 1C and 1175 1C, respectively, in covered alumina crucibles for 2 h in air with a heating rate of 5 1C/min. For electrical measurements, a silver paste was screenprinted on both sides of each specimen, fired at 700 1C for 30 min, and then poled in silicone oil bath at 80 1C under a direct electric field of 50 kV/cm for 15 min. The crystal structures of the poled and unpoled samples were analyzed with an X-ray diffractometer (XRD, RAD III, Rigaku, Japan) using Cu Kα radiation. The relative density of the fired specimen was determined by the Archimedes method. A field-emission scanning electron microscope (FE-SEM, JEOL, JSM-65OFF, Japan) was used to examine the surface morphology of samples. The electrical polarization (P) and electromechanical strain (S) as a function of external electric field (E) were recorded at 0.3 Hz with a 15 mF measurement capacitance using a Sawyer-Tower circuit equipped with an optical sensor (Philtec, Inc., Annapolis, MD, USA). The piezoelectric constant d33 was measured using a Berlincourt d33-meter after poling samples under a direct electric field of 50 kV/cm for 15 min in silicone oil kept at 80 1C. The planar piezoelectric coupling coefficient (kp) and electromechanical quality factor (Qm) were characterized by the resonanceantiresonance method. 3. Results and discussion Field-emission scanning electron microscopic investigations were carried out to study grain size and grain morphology of Li100x and La100x, and the results are shown in Fig. 1. All Fig. 1. Comparison of scanning electron micrographs between Li- and La-modified BNKT ceramics with different dopant levels. S460 T.H. Dinh et al. / Ceramics International 41 (2015) S458–S463 samples show a similar grain morphology and dense microstructures like previous reports on modified BNKT ceramics [7,8,9,23,24]. As a function of doping level, the grain size of both Li100x and La100x ceramics were increased slightly. The increase in grain size of KNN–LiTaO3 [25] and BNT–KNN [26] by added Li þ were also presented. The increased sinterability was also observed in BNKT ceramics doped with Zr [23], Hf [24], Nb [7], and co-doped with Li and Ta [11]. In addition, the lower sintering temperature for Li-doped BNKT was also reported on (Na1 x yKxLiy)0.5Bi0.5TiO3 [27], which was sintered at 1040– 1120 1C in air. The acceptor dopants were known to enhance interdiffusions during sintering via generation of O-vacancies [22]. XRD patterns of all sintered specimens in the 2θ range of 39–481 are presented in Fig. 2. A single phase perovskite structure without any traces of secondary phases was observed for all compositions. It was reported [5–13] that the difference between rhombohedral and tetragonal structures in the perovskite materials can be easily distinguished by the {111} and {200} profiles of XRD patterns. As observed in Fig. 2(a) and (b), the addition of either Li or La induced a significant change in the crystal structure. With increasing x, Li100x and La100x revealed a phase transition from the coexistence of rhombohedral and tetragonal to pseudocubic phases, which might have been arisen from the size difference between the substituent and lattice ions. The occupation of Li þ and La3 þ ions at A-site tends to shrink the lattice owing to the formation of oxygen and A-site vacancies and a smaller ionic size of Li þ and La3 þ than that of K þ and Na þ (ionic radii: 1.39, 1.64, 1.36, and 0.92 A1 for Na þ , K þ , La3 þ , and Li þ ; CN ¼ 12 [28]). The effects of Li and La doping on the crystal structure of BNKT ceramics show similar tendency to that of Zr [23], Nb [4], and Sn [9] doping. In addition, the systematic XRD investigation of unpoled (Fig. 2(a)) and poled (Fig. 2(c)) Li100x samples was carried out. The phase transition from mixture of rhombohedral and tetragonal phases to a pseudocubic phase occurred for unpoled specimens at x around 0.03 while for poled samples with x higher than 0.02, rhombohedral phase was observed. It is suggested that during the poling process as well as under applying electric field, the pseudocubic phase of Li100x ceramics with x higher than 0.02 was not stable and transformed to rhombohedral phase. This behavior is in good agreement with the lack of negative strain in bipolar electric field induced strain curves as well as negligible remnant polarization in the P–E hysteresis loops, which are discussed below. Polarization versus electric field hysteresis loops of Li- and La-doped BNKT were measured at a frequency of 0.3 Hz at room temperature and the results are shown in Fig. 3. A saturated square hysteresis loop was observed for ceramics with low dopant levels, indicating a relatively large remnant polarization (Pr) as well as coercive field (Ec). In case of Li doping, the saturated P–E loop was maintained up to x ¼ 0.05 while La doping brought about gradual slimming in the P–E loop with increasing doping level. The effect of dopant level on coercive field, remnant polarization, piezoelectric constant, and mechanical quality factor of BNKT-based ceramics are compared in Fig. 4 for Li and La doped specimens. Li doping seems to induce hardening of BNKT by generation of O-vacancies to maintain charge neutrality in the lattice [29]. It has been known that oxygen vacancies is one of the main reasons of reducing the domainwall motion [22,26,30,31], resulting in higher Ec (Fig. 4(a)) of Li100x ceramics. On the other hand, the drastic decreases in Pr (Fig. 4(b)) and Ec (Fig. 4(a)) of La-doped BNKT ceramics could be attributed to ferroelectric-relaxor phase transition, which was olso observed in BNKT doped ceramics doped with Zr, Hf, Nb, Sn, and Ta [7,8,9,23,24]. The highest d33 value (172 pC/N) was observed in La2 and an improved Qm (253) was measured for Li2, as presented in Fig. 4(c) and (d). These Fig. 2. XRD patterns as a function of doping level: (a) Li100x, (b) La100x, and (c) Poled-Li100x; x¼ 0–0.05. T.H. Dinh et al. / Ceramics International 41 (2015) S458–S463 S461 Fig. 3. Comparison of Li- and La-doping effects on the P–E hysteresis loop of BNKT ceramics. Fig. 4. Effect of doping level on (a) the coercive field (Ec), (b) remnant polarization (Pr), (c) piezoelectric constant (d33), and (d) mechanical quality factor (Qm) of Li- and La-doped BNKT ceramics. Fig. 5. Effect of dopant content on the bipolar S–E hysteresis loops of BNKT ceramics. observations can be explained based on the hardening and softening effect of acceptor and donor doping on BNKT-based ceramics, respectively [22,29]. Fig. 5 shows bipolar electric-field-induced strain loops of Liand La-doped BNKT ceramics. An unmodified BNKT exhibited a butterfly-shaped strain curve, which has been typically observed in ferroelectric materials. With increasing the dopant content, the negative strain, Sneg of Li100x ceramics maintained almost constant, however, that of La100x specimens decreased. From the S–E loops, both Sneg and maximum bipolar strain/electric field (d n33 ) as a function of dopant content were determined and plotted in Fig. 6. A significant difference between two different dopants can be seen in composition dependence of negative strain, Sneg (Fig. 6(a)) and converse piezoelectric constant dn33 (Fig. 6(b)). The existence of considerable Sneg at both þ Ec and –Ec implies that there are ferroelectric domains whose orientations reversed when the external field is reversed. It is seen in Fig. 6 that La-doping leads to an abrupt drop in the Sneg at x¼ 0.03, while Sneg is insensitive to doping level for Li-doped specimens. This observation is also S462 T.H. Dinh et al. / Ceramics International 41 (2015) S458–S463 Table 1 Ferroelectric and electromechanical properties of Li100x and La100x ceramics; x¼ 0–0.05. Composition Pr (μC/cm2) Ec (kV/cm) d33 (pC/N) Qm kp (%) Smax/Emax (pm/V) Li1 Li2 Li3 Li4 Li5 La0 La1 La2 La3 La4 La5 22 20 21 19 19 19 20 17 2 1 0.5 33 34 35 36 36 36 33 21 7 3 0.5 114 112 110 103 105 130 156 172 5 2 2 214 253 208 172 166 165 110 51 – – – 31 38 34 33 33 31 31 29 – – – 216 233 250 216 233 250 250 300 650 400 216 Fig. 6. Variation of (a) negative strains (Sneg) and (b) converse piezoelectric constant (d33) as a function of A-site doping levels. Acknowledgments consistent with the results observed in the P–E loops in Fig. 3, and also supports the fact that La-doping induces the ferroelectricrelaxor phases transition in BNKT. It should be pointed out that a large strain enhancement is observed when Sneg abruptly decreases when 3 mol% La is doped, where the highest Smax/Emax of 650 pm/V is also attained as can be seen in Fig. 6(b) [32]. Similar phenomena were also observed in BNKT ceramics doped/modified with Zr [23], Hf [24], Nb [7], Sn [9], Ta [8], LiTaO3 [11], SrTiO3 [33], (K0.5Na0.5)NbO3 [34], and Sr(K1/4Nb3/4)O3 [35]. The various ferroelectric and electromechanical properties of Li100x and La100x ceramics with x¼ 0.00–0.05 are summarized in Table 1. It should be noted that the highest Qm and kp values were measured for Li2, which were 253 and 38%, respectively. The bipolar Smax/Emax (dn33 ) reached 650 pm/V at 60 kV/cm in La3 and the highest d33 was measured as 172 pC/N for La2. 4. Conclusions This work systematically compared the effects of Li- and La-doping on the crystal structure, microstructure and electromechanical properties of lead-free BNKT ceramics. Two dopants showed definite differences in terms of ferroelectric and strain properties. Li doping resulted in hardening of BNKT that was evidenced by the increased ferroelectricity as well as mechanical quality factor. On the contrary, La doping induced a ferroelectric-relaxor phase transition when 3 mol% La was doped, where an abnormal increase in the strain was observed like previous reports on B-site donor doped BNKT. The present work is believed to be meaningful in view of experimental demonstration of definite differences in the effects between A-site acceptor and donor doping on the material properties of Bi-based perovskite ceramics. Conflict of interest We declare that we do not have any commercial or associative interest that represents a conflict of interest in connection with the work submitted. This work was supported by the National Research Foundation of Korea (NRF) Grant (2013R1A1A2058917). M.R. Bafandeh thanks the financial support of the University of Kashan. References [1] A. Sasaki, T. Chiba, Y. Mamiya, E. Otsuki, Dielectric and piezoelectric properties of (Bi,Na)TiO3–BaTiO3–BiFeO3 systems, Jpn. J. Appl. Phys. 38 (9B) (1999) 5564–5567. [2] H. Ishii, H. Nagata, T. Takenaka, Morphotropic phase boundary and electrical properties of bismuth sodium titanate–potassium niobate solidsolution ceramics, Jpn. J. Appl. Phys. 40 (2001) 5660–5663. [3] K. Yoshii, Y. Hiruma, H. Nagata, T. Takenaka, Electrical properties and depolarization temperature of (Bi1/2Na1/2)TiO3–(Bi1/2K1/2)TiO3 lead-free piezoelectric ceramics, Jpn. J. Appl. Phys. 45 (5B) (2006) 4493–4496. [4] Y. Zhang, R. Chu, Z. Xu, J. Hao, Q. Chen, F. Peng, W. Li, G. Li, Q. Yin, Piezoelectric and dielectric properties of Sm2O3-doped 0.82Bi0.5Na0.5TiO3–0.18Bi0.5K0.5TiO3 ceramics, J. Alloy. Compd. 502 (2010) 341–345. [5] A. Ullah, C.W. Ahn, A. Hussain, S.Y. Lee, H.J. Lee, I.W. Kim, Phase transition and large electric field induced strain in BiAlO3-modified Bi0.5(Na,K)0.5TiO3 lead free piezoelectric ceramics, Curr. Appl. Phys. 10 (2010) 1174–1181. [6] Z.C. Rong, C.L. Yuan, Dielectric and piezoelectric properties of Bi0.5(Na0.82K0.18)0.5TiO3–LiSbO3 lead-free piezoelectric ceramics, Bull. Mater. Sci. 34 (2011) 933–936. [7] K.N. Pham, A. Hussain, C.W. Ahn, I.W. Kim, S.J. Jeong, J.S. Lee, Giant strain in Nb-doped Bi0.5(Na0.82K0.18)0.5TiO3 lead free piezoelectric ceramics, Mater. Lett. 64 (2010) 2219–2222. [8] N.B. Do, H.B. Lee, C.H. Yoon, J.K. Kang, J.S. Lee, I.W. Kim, Effect of Ta-substitution on the ferroelectric and piezoelectric properties of Bi1/ 2(Na0.82K0.18)1/2TiO3 ceramics, Trans. Electr. Electron. Mater. 12 (2011) 64–67. [9] J.S. Lee, K.N. Pham, H.S. Han, H.B. Lee, V.D.N. Tran, Strain enhancement of lead-free Bi1/2(Na0.82K0.18)1/2TiO3 piezoelectric ceramics by Sn doping, J. Korean Phys. Soc. 60 (2012) 212–215. [10] H.S. Han, W. Jo, J.K. Kang, C.W. Ahn, I.W. Kim, K.K. Ahn, J.S. Lee, Incipient piezoelectric and electrostriction behavior in Sn-doped BNT– BKT lead-free ceramics, J. Appl. Phys. 113 (2013) 154102. [11] V.Q. Nguyen, H.S. Han, K.J. Kim, D.D. Dang, K.K. Ahn, J.S. Lee, Strain enhancement in Bi1/2(Na0.82K0.18)1/2TiO3 lead-free electromechanical ceramics by co-doping with Li and Ta, J. Alloy. Compd. 511 (2012) 237–241. T.H. Dinh et al. / Ceramics International 41 (2015) S458–S463 [12] H.S. Han, W. Jo, J. Rödel, I.K. Hong, W.P. Tai, J.S. Lee, Coexistence of ergodicity and nonergodicity in LaFeO3-modified Bi1/2(Na0.78K0.22)1/ 2TiO3 relaxor, J. Phys.: Condens. Matter 24 (2012) 365901. [13] T.H. Dinh, H.Y. Lee, C.H. Yoon, R.A. Malik, Y.M. Kong, J.S. Lee, Effect of lanthanum doping on structural ferroelectric and strain properties of Bi1/2(Na0.82K0.18)1/2TiO3 lead free ceramics, J. Korean Phys. Soc. 62 (2013) 1004–1008. [14] A. Zaman, Y. Iqbal, A. Hussain, M.H. Kim, R.A. Malik, Dielectric, ferroelectric, and field-induced strain properties of Ta-doped 0.99Bi0.5(Na0.82K0.18)0.5TiO3–0.01LiSbO3 ceramics, J. Mater. Sci. 49 (2014) 3205–3214. [15] M.I. Morozov, D. Damjanovic, Hardening-softening transition in Fedoped Pb(Zr,Ti)O3 ceramics and evolution of the third harmonic of the polarization response, J. Appl. Phys. 104 (2008) 034107. [16] M.I. Morozov, D. Damjanovic, Charge migration in Pb(Zr,Ti)O3 ceramics and its relation to ageing, hardening, and softening, J. Appl. Phys. 107 (2010) 034106. [17] D. Viehland, Effect of uniaxial stress upon the electromechanical properties of various piezoelectric ceramics and single crystals, J. Am. Ceram. Soc. 89 (2006) 775–785. [18] B. Jaffe, W. Cook, H. Jaffe, Piezoelectric Ceramics, Academic, London, 1971, p. 101. [19] A. Chandrasekaran, D. Damjanovic, N. Setter, N. Marzari, Defect ordering and defect-domain-wall interactions in PbTiO3: a firstprinciples study, Phys. Rev. B 88 (2013) 214116. [20] H.G. Yeo, Y.S. Sung, T.K. Song, J.H. Cho, M.H. Kim, Donor doping effects on the ferroelectric and the piezoelectric properties of Pb-free (Bi0.5Na0.5)TiO3 ceramics, J. Korean Phys. Soc. 54 (2009) 896–900. [21] H.S. Han, C.W. Ahn, I.W. Kim, A. Hussain, J.S. Lee, Destabilization of ferroelectric order in bismuth perovskite ceramics by A-site vacancies, Mater. Lett. 70 (2012) 98–100. [22] E. Taghaddos, M. Hejazi, A. Safari, Electromechanical properties of acceptor-doped lead-free piezoelectric ceramics, J. Am. Ceram. Soc. 97 (2014) 1756–1762. [23] A. Hussain, C.W. Ahn, J.S. Lee, A. Ullar, I.W. Kim, Large electric-fieldinduced strain in Zr-modified lead-free Bi0.5(Na0.75K0.25)0.5TiO3 piezoelectric ceramics, Sens. Actuators A: Phys. 158 (2010) 84–89. S463 [24] A. Hussain, C.W. Ahn, A. Ullar, J.S. Lee, I.W. Kim, The effect of hafnium substitution on dielectric and piezoelectric properties of lead-free Bi0.5(Na0.78K0.22)0.5(Ti1 xHfx)O3 ceramics, Jpn. J. Appl. Phys. 49 (2010) 041054. [25] M.S. Kim, S.J. Jeong, J.S. Song, Microstructures and piezoelectric properties in the Li2O-excess 0.95(Na0.5K0.5)NbO3–0.05LiTaO3 ceramics, J. Am. Ceram. Soc. 90 (2007) 3338–3340. [26] S. Wongsaenmai, R. Yimnirun, P. Laoratanakul, Effects of dopants on phase formation and microstructure of bismuth sodium titanate–potassium sodium niobate ceramics, Ferroelectrics 458 (2014) 214–220. [27] W. Lu, Y. Wang, G. Fan, X. Wang, F. Liang, The structural and electric properties of Li- and K-substituted Bi0.5Na0.5TiO3 ferroelectric ceramics, J. Alloy. Compd. 509 (2011) 2738–2744. [28] R.D. Shannon, Crystal physics, diffraction, theoretical and general crystallography, Acta Crystallogr. A 32 (1976) 751–767. [29] J. Li, F. Wang, C.M. Leung, S.W. Or, Y. Tang, X. Chen, T. Wang, X. Qin, W. Shi, Large strain response in acceptor- and donor-doped Bi0.5Na0.5TiO3-based lead-free ceramics, J. Mater. Sci. 46 (2011) 5702–5708. [30] S.E. Park, S.J. Chung, Ferroic phase transition in (Na1/2Bi1/2)TiO3 crystals, J. Am. Ceram. Soc. 79 (1996) 1290–1296. [31] U. Robels, L. Scheneider-Stormanm, G. Arlt, Domain wall trapping as a results of internal bias fields, Ferroelectrics 133 (1992) 223–228. [32] W. Jo, T. Granzow, E. Aulback, J. Rödel, D. Damjanovic, Origin of the large strain response in (K0.5Na0.5)NbO3-modified (Bi0.5Na0.5)TiO3– BaTiO3 lead-free piezoceramics, J. Appl. Phys. 105 (2009) 094102. [33] K. Wang, A. Hussain, W. Jo, J. Rödel, Temperature-dependent properties of (Bi1/2Na1/2)TiO3–(Bi1/2K1/2)TiO3-SrTiO3 lead-free piezoceramics, J. Am. Ceram. Soc. 95 (2012) 2241–2247. [34] K.T.P. Seifert, W. Jo, J. Rödel, Temperature-insensitive large strain of (Bi1/2Na1/2)TiO3–(Bi1/2K1/2)TiO3–(K0.5Na0.5)NbO3 lead-free piezoceramics, J. Am. Ceram. Soc. 93 (2010) 1392–1396. [35] V.D.N. Tran, H.S. Han, C.H. Yoon, J.S. Lee, W. Jo, J. Rödel, Thermal stable field-induced strain of lead-free electrostrictive Bi-based perovskite ceramics, Mater. Lett. 65 (2011) 2607–2609.