Abstract
Yttrium substitution in \(\hbox {Ba}(\hbox {Zr}_x \hbox {Ti}_{1-x})\hbox {O}_3\) (BZT) solid solutions has been found to be an effective way to induce relaxor behavior and improve their dielectric and ferroelectric performances. However, the underlying mechanism of such enhancement is not yet well understood. Here we employ density functional theory with the generalized gradient approximation to investigate the effect of yttrium on the structural and electronic properties of BZT for x = 0.125, 0.250, and 0.375. The results will be discussed in terms of yttrium site preference, atomic pair distribution functions (PDFs), cation off-centering and electronic density of states. It was found that yttrium incorporation could occur in either A- or B-site with corresponding defect vacancies and that the effect of the sites of impurities is only to cause small changes in formation energies. The calculated PDFs and cation off-centering indicate that yttrium ions actively induce lattice distortion and increase structural disorder. This implies that the addition of yttrium in BZT suppresses the ferroelectric instabilities and may help to explain the transition from ferroelectric to relaxor state of such materials.
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Data availability
Ionic coordinates generated during this study are deposited in the Figshare repository (https://www.doi.org/10.6084/m9.figshare.6969515). All other data are available from the authors upon request.
References
P.W. Rehrig, S.E. Park, S.T. McKinstry, G.L. Messing, B. Jones, T.R. Shrout, Piezoelectric properties of zirconium-doped barium titanate single crystals grown by templated grain growth. J. Appl. Phys. 86(3), 1657 (1999). https://doi.org/10.1063/1.370943
Z. Yu, R. Guo, A.S. Bhalla, Orientation dependence of the ferroelectric and piezoelectric behavior of \(\text{Ba} (\text{Ti}_{1-x} \text{Zr}_x)\text{O}_3\) single crystals. Appl. Phys. Lett. 77(10), 1535 (2000). https://doi.org/10.1063/1.1308276
Z. Yu, C. Ang, R. Guo, A.S. Bhalla, Piezoelectric and strain properties of \(\text{Ba} (\text{Ti}_{1-x} \text{Zr}_x)\text{O}_3\) ceramics. J. Appl. Phys. 92(3), 1489 (2002). https://doi.org/10.1063/1.1487435
X. Chou, J. Zhai, X. Yao, Relaxor behavior and dielectric properties of \(\text{La}_2 \text{O}_3\)-doped barium zirconium titanate ceramics for tunable device applications. Mater. Chem. Phys. 109(1), 125 (2008). https://doi.org/10.1016/j.matchemphys.2007.11.005
S. Piskunov, E. Heifets, R. Eglitis, G. Borstel, Bulk properties and electronic structure of \(\text{SrTiO}_3\), \(\text{BaTiO}_3\), \(\text{PbTiO}_3\) perovskites: an ab initio HF/DFT study. Comput. Mater. Sci. 29(2), 165 (2004). https://doi.org/10.1016/j.commatsci.2003.08.036
A. Chassé, S. Borek, K.M. Schindler, M. Trautmann, M. Huth, F. Steudel, L. Makhova, J. Gräfe, R. Denecke, High-resolution X-ray absorption spectroscopy of \(\text{BaTiO}_{3}\): experiment and first-principles calculations. Phys. Rev. B 84, 195135 (2011). https://doi.org/10.1103/PhysRevB.84.195135
Q.J. Liu, N.C. Zhang, F.S. Liu, H.Y. Wang, Z.T. Liu, \(\text{BaTiO}_3\): Energy, geometrical and electronic structure, relationship between optical constant and density from first-principles calculations. Opt. Mater. 35(12), 2629 (2013). https://doi.org/10.1016/j.optmat.2013.07.034
D.H. Kim, H.S. Kwok, Pulsed laser deposition of \(\text{BaTiO}_3\) thin films and their optical properties. App. Phys. Lett. 67(13), 1803 (1995). https://doi.org/10.1063/1.115064
A. Garca, D. Vanderbilt, Electromechanical behavior of \(\text{BaTiO}_3\) from first principles. App. Phys. Lett. 72(23), 2981 (1998). https://doi.org/10.1063/1.121514
M.G. Stachiotti, Ferroelectricity in \(\text{BaTiO}_3\) nanoscopic structures. App. Phys. Lett. 84(2), 251 (2004). https://doi.org/10.1063/1.1637142
G.H. Kwei, A.C. Lawson, S.J.L. Billinge, S.W. Cheong, Structures of the ferroelectric phases of barium titanate. J. Phys. Chem. 97(10), 2368 (1993). https://doi.org/10.1021/j100112a043
I. Levin, T.G. Amos, S.M. Bell, L. Farber, T.A. Vanderah, R.S. Roth, B.H. Toby, Phase equilibria, crystal structures, and dielectric anomaly in the \(\text{BaZrO}_3\)-\(\text{CaZrO}_3\) system. J. Solid State Chem. 175(2), 170 (2003). https://doi.org/10.1016/S0022-4596(03)00220-2
J.W. Bennett, I. Grinberg, A.M. Rappe, Effect of symmetry lowering on the dielectric response of \({\rm BaZrO}_{3}\). Phys. Rev. B 73, 180102 (2006). https://doi.org/10.1103/PhysRevB.73.180102
T. Tsurumi, Y. Yamamoto, H. Kakemoto, S. Wada, H. Chazono, H. Kishi, Dielectric properties of \(\text{BaTiO}_3\)–\(\text{BaZrO}_3\) ceramics under a high electric field. J. Mater. Res. 17(4), 755759 (2002). https://doi.org/10.1557/JMR.2002.0110
R. Farhi, M. El Marssi, A. Simon, J. Ravez, A raman and dielectric study of ferroelectric \(\text{Ba} (\text{Ti}_{1-x} \text{Zr}_x)\text{O}_3\) ceramics. Eur. Phys. J. B 9(4), 599 (1999). https://doi.org/10.1007/s100510050803
J. Ravez, C. Broustera, A. Simon, Lead-free ferroelectric relaxor ceramics in the \(\text{BaTiO}_3\)–\(\text{BaZrO}_3\)–\(\text{CaTiO}_3\) system. J. Mater. Chem. 9, 1609 (1999). https://doi.org/10.1039/A902335F
T. Maiti, R. Guo, A.S. Bhalla, Structure-property phase diagram of \(\text{BaZr}_x \text{Ti}_{1-x} \text{O}_3\) system. J. Am. Ceram. Soc. 91(6), 1769 (2008). https://doi.org/10.1111/j.1551-2916.2008.02442.x
A. Simon, J. Ravez, M. Maglione, The crossover from a ferroelectric to a relaxor state in lead-free solid solutions. J. Phys. Condens. Matter 16(6), 963 (2004)
S. Ke, H. Fan, H. Huang, H.L.W. Chan, S. Yu, Dielectric dispersion behavior of \(\text{Ba} (\text{Zr}_x \text{Ti}_{1-x})\text{O}_3\) solid solutions with a quasiferroelectric state. J. Appl. Phys. 104(3), 034108 (2008). https://doi.org/10.1063/1.2964088
S.Y. Liu, E. Zhang, S. Liu, D.J. Li, Y. Li, Y. Liu, Y. Shen, S. Wang, Composition- and pressure-induced relaxor ferroelectrics: first-principles calculations and landau-devonshire theory. J. Am. Ceram. Soc. 99(10), 3336 (2016). https://doi.org/10.1111/jace.14350
S.Y. Liu, Y. Meng, S. Liu, D.J. Li, Y. Li, Y. Liu, Y. Shen, S. Wang, Compositional phase diagram and microscopic mechanism of \(\text{Ba}_{1-x} \text{Ca}_x \text{Zr}_y \text{Ti}_{1-y} \text{O}_3\) relaxor ferroelectrics. Phys. Chem. Chem. Phys. 19, 22190 (2017). https://doi.org/10.1039/C7CP04530A
C. Ostos, L. Mestres, M. Martnez-Sarrin, J. Garca, A. Albareda, R. Perez, Synthesis and characterization of a-site deficient rare-earth doped \(\text{BaZr}_x \text{Ti}_{1-x} \text{O}_3\) perovskite-type compounds. Solid State Sci. 11(5), 1016 (2009). https://doi.org/10.1016/j.solidstatesciences.2009.01.006
L. Gao, J. Zhai, Y. Zhang, X. Yao, Influence of rare-earth addition on dielectric properties and relaxor behavior of barium zirconium titanate thin films. J. Appl. Phys. 107(6), 064105 (2010). https://doi.org/10.1063/1.3330753
X. Chou, J. Zhai, H. Jiang, X. Yao, Dielectric properties and relaxor behavior of rare-earth (La, Sm, Eu, Dy, Y) substituted barium zirconium titanate ceramics. J. Appl. Phys. 102(8), 084106 (2007). https://doi.org/10.1063/1.2799081
X. Diez-Betriu, J. Garcia, C. Ostos, A. Boya, D. Ochoa, L. Mestres, R. Perez, Phase transition characteristics and dielectric properties of rare-earth (La, Pr, Nd, Gd) doped \(\text{Ba} (\text{Zr}_{0.09} \text{Ti}_{0.91})\text{O}_3\) ceramics. Mater. Chem. Phys. 125(3), 493 (2011). https://doi.org/10.1016/j.matchemphys.2010.027
S. Ghosh, S. Rout, Induced instability in local structure and ferroelectric polarization of rare earth modified BZT relaxor ceramics. Curr. Appl. Phys. 16(9), 989 (2016). https://doi.org/10.1016/j.cap.2016.05.018
S.B. Reddy, K.P. Rao, M.R. Rao, Effect of La substitution on the structural and dielectric properties of BaZr0.1Ti0.9O3 ceramics. J Alloys Compd. 481(1), 692 (2009). https://doi.org/10.1016/j.jallcom.2009.03.075
D. Shan, Y. Qu, J. Song, Dielectric properties and substitution preference of yttrium doped barium zirconium titanate ceramics. Solid State Commun. 141(2), 65 (2007). https://doi.org/10.1016/j.ssc.2006.09.050
T. Badapanda, L.S. Cavalcante, G.E. da Luz, N.C. Batista, S. Anwar, E. Longo, Effect of yttrium doping in barium zirconium titanate ceramics: a structural, impedance, and modulus spectroscopy study. Metall. Mater. Tran. A 44(9), 4296 (2013). https://doi.org/10.1007/s11661-013-1770-3
T. Badapanda, S.K. Rout, L.S. Cavalcante, J.C. Sczancoski, S. Panigrahi, T.P. Sinha, E. Longo, Structural and dielectric relaxor properties of yttrium-doped \(\text{Ba} (\text{Zr}_{0.25} \text{Ti}_{0.75})\text{O}_3\) ceramics. Mater. Chem. Phys. 121(1), 147 (2010). https://doi.org/10.1016/j.matchemphys.2010.01.008
P.A. Jha, A. Jha, Effects of yttrium substitution on structural and electrical properties of barium zirconate titanate ferroelectric ceramics. Curr. Appl. Phys. 13(7), 1413 (2013). https://doi.org/10.1016/j.cap.2013.04.032
P.K. Patel, K. Yadav, Effect of yttrium on microstructure, dielectric, ferroelectric and optical properties of BaZr0.10Ti0.90O3 nanoceramics. Phys. B Condens. Matter 442, 39 (2014). https://doi.org/10.1016/j.physb.2014.02.020
X.Y. Zhao, Y.H. Wang, M. Zhang, N. Zhao, S. Gong, Q. Chen, First-principles calculations of the structural, electronic and optical properties of \(\text{BaZr}_x \text{Ti}_{1-x} \text{O}_3\) ( \(x = 0\), 0.25, 0.5, 0.75). Chin. Phys. Lett. 28(6), 067101 (2011)
P. Erhart, K. Albe, Thermodynamics of mono- and di-vacancies in barium titanate. J. Appl. Phys. 102(8), 084111 (2007). https://doi.org/10.1063/1.2801011
S. Körbel, C. Elsässer, Ab initio and atomistic study of ferroelectricity in copper-doped potassium niobate. Phys. Rev. B 84, 014109 (2011). https://doi.org/10.1103/PhysRevB.84.014109
D. Vanderbilt, Soft self-consistent pseudopotentials in a generalized eigenvalue formalism. Phys. Rev. B 41, 7892 (1990). https://doi.org/10.1103/PhysRevB.41.7892
P. Giannozzi, QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials. J. Phys. Condens. Matter 21(39), 395502 (2009). http://www.quantum-espresso.org
J.P. Perdew, K. Burke, M. Ernzerhof, Generalized gradient approximation made simple. Phys. Rev. Lett. 77, 3865 (1996). https://doi.org/10.1103/PhysRevLett.77.3865
H.J. Monkhorst, J.D. Pack, Special points for Brillouin-zone integrations. Phys. Rev. B 13, 5188 (1976). https://doi.org/10.1103/PhysRevB.13.5188
P.E. Blöchl, O. Jepsen, O.K. Andersen, Improved tetrahedron method for Brillouin-zone integrations. Phys. Rev. B 49, 16223 (1994). https://doi.org/10.1103/PhysRevB.49.16223
P. Haas, F. Tran, P. Blaha, Calculation of the lattice constant of solids with semilocal functionals. Phys. Rev. B 79, 085104 (2009). https://doi.org/10.1103/PhysRevB.79.085104
R.D. Shannon, Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides. Acta Crystallogr. Sect. A 32(5), 751 (1976). https://doi.org/10.1107/S0567739476001551
I.K. Jeong, C.Y. Park, J.S. Ahn, S. Park, D.J. Kim, Ferroelectric-relaxor crossover in \(\text{Ba}({\text{Ti}}_{1-x}{\text{Zr}}_{x}) {\text{O}}_{3}\) studied using neutron total scattering measurements and reverse monte carlo modeling. Phys. Rev. B 81, 214119 (2010). https://doi.org/10.1103/PhysRevB.81.214119
C. Laulhé, F. Hippert, R. Bellissent, A. Simon, G.J. Cuello, Local structure in \({\text{BaTi}}_{1-x}{\text{Zr}}_{x}{\text{O}}_{3}\) relaxors from neutron pair distribution function analysis. Phys. Rev. B 79, 064104 (2009). https://doi.org/10.1103/PhysRevB.79.064104
R. Kagimura, M. Suewattana, D.J. Singh, (Ba, K, La)\({\text{ZrO}}_{3}\) as a possible lead-free ferroelectric: density functional calculations. Phys. Rev. B 78, 012103 (2008). https://doi.org/10.1103/PhysRevB.78.012103
A. Yamanaka, M. Kataoka, Y. Inaba, K. Inoue, B. Hehlen, E. Courtens, Evidence for competing orderings in strontium titanate from hyper-Raman scattering spectroscopy. Europhys. Lett. 50(5), 688 (2000). https://doi.org/10.1209/epl/i2000-00325-6
A. Singh, A. Senyshyn, H. Fuess, D. Pandey, Ferroelectric and antiferrodistortive phase transition in the multiferroic (\(\text{Bi}_{0.8} \text{Ba}_{0.2}\))(\(\text{Fe}_{0.8} \text{Ti}_{0.2})\text{O}_3\): A high temperature neutron powder diffraction study. J. Appl. Phys. 110(2), 024111 (2011). https://doi.org/10.1063/1.3606500
R. Ranjan, D. Pandey, N.P. Lalla, Novel features of \({\rm Sr}_{1-x}{\rm Ca}_{x} {\rm TiO}_{3}\) phase diagram: evidence for competing antiferroelectric and ferroelectric interactions. Phys. Rev. Lett. 84, 3726 (2000). https://doi.org/10.1103/PhysRevLett.84.3726
A.N. Morozovska, E.A. Eliseev, M.D. Glinchuk, L.Q. Chen, V. Gopalan, Interfacial polarization and pyroelectricity in antiferrodistortive structures induced by a flexoelectric effect and rotostriction. Phys. Rev. B 85, 094107 (2012). https://doi.org/10.1103/PhysRevB.85.094107
Acknowledgements
We acknowledge the financial support from the Thailand Research Fund and the Department of Physics, Mahidol University. The authors would like to thank W. Singsomroj and K. Matan for useful discussion.
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Thammada, W., Suewattana, M. First-principle study of local and electronic structures of yttrium-doped \(\hbox {Ba}(\hbox {Zr}_x \hbox {Ti}_{1-x}) \hbox {O}_3\). Appl. Phys. A 124, 644 (2018). https://doi.org/10.1007/s00339-018-2063-x
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DOI: https://doi.org/10.1007/s00339-018-2063-x