Abstract
Thin films of Pb(Sc1/2Ta1/2)O3 (PST) were fabricated using an optimized chemical solution deposition procedure involving the de-hydration of scandium acetate and the addition of up to 30% excess lead in solution. The choice of substrate was found to impact the thermal induced stress in the films as confirmed by wafer bending and in-plane grazing angle x-ray diffraction measurements. The presence of either a compressive or a tensile in-plane stress led to a reduction in the temperature of the dielectric maximum, whereas the value of the dielectric maximum remained relatively unchanged; its value reduced by an order of magnitude compared with ceramic samples. It is concluded that mechanical stress alone is not the sole factor in the reduction of PST thin film permittivity. Microstructural features resulting from processing induced defects or an incomplete transformation to the relaxor state may be responsible for this commonly observed phenomenon.
Similar content being viewed by others
References
S.E. Park and T.S. Shrout: Ultrahigh strain and piezoelectric behavior in relaxor based ferroelectric single crystals. J. Appl. Phys. 82, 1804 (1997).
Z. Kighelman, D. Damjanovic, and N. Setter: Electromechanical properties and self-polarization in relaxor Pb(Mg1/3Nb2/3)O3 thin films. J. Appl. Phys. 89, 1393 (2001).
L. Francis, Y. Oh, and D. Payne: Sol-gel processing and properties of lead magnesium niobate powders and thin-layers. J. Mater. Sci. 25, 5007 (1990).
J. Park and S. Trolier-McKinstry: Dependence of dielectric and piezoelectric properties on film thickness for highly 100-oriented lead magnesium niobate-lead titanate (70/30) thin films. J. Mater. Res. 16, 268 (2001).
B.J. Kuh, W.K. Choo, K. Brinkman, D. Damjanovic, and N. Setter: Dielectric and piezoelectric properties of relaxor Pb(Sc1/2Nb1/2)O3 thin films. Appl. Phys. Lett. 83, 1614 (2003).
M. Tyunina and J. Levoska: Dielectric nonlinearity in relaxor and ferroelectric thin films of chemically ordered PbSc0.5Nb0.5O3. Appl. Phys. Lett. 85, 4720 (2004).
D. Liu and D. Payne: Lower temperature crystallization and ordering in sol-gel derived Pb(Sc0.5Ta0.5)O3 powders and thin-layers. J. Appl. Phys. 77, 3361 (1995).
Z. Huang, P. Donohue, Q. Zhang, D. Williams, C. Anthony, M. Todd, and R. Whatmore: Comparative studies of PST thin films as prepared by sol-gel, LDCVD and sputtering techniques. Integrated Ferroelectrics 45, 79 (2002).
K. Brinkman, M. Cantoni, A. Tagantsev, P. Muralt, and N. Setter: Dielectric response and structural features of Pb(Sc1/2Ta1/2)O3 (PST) sol-gel derived thin films. J. Electroceram. 13, 105 (2004).
S. Kamba, M. Berta, M. Kempa, J. Petzelt, K. Brinkman, and N. Setter: Far-infrared soft-mode behavior in Pb(Sc1/2Ta1/2)O3 thin films. J. Appl. Phys. 98, 074103 (2005).
S. Kamba, M. Kempa, V. Bovtun, J. Petzelt, K. Brinkman, and N. Setter: Soft and central mode behaviour in Pb(Mg1/3Nb2/3)O3 relaxor ferroelectric. J. Phys.: Condens. Matter 17, 3965 (2005).
R. Ramesh, S. Aggarwa, and O. Auciello: Science and technology of ferroelectric films and heterostructures for non-volatile ferroelectric memories. Mater. Sci. Eng. 32, 191 (2001).
B. Nagaraj, S. Aggarwal, T.K. Song, T. Sawhney, and R. Ramesh: Leakage current mechanisms in lead-based thin film ferroelectric capacitors. Phys. Rev. B 59, 16022 (1999).
M. Dawber, K. Rabe, and J. Scott: Physics of thin-film ferroelectric oxides. Rev. Mod. Phys. 77, 1083 (2005).
X. Ren: Large electric-field-induced strain in ferroelectric crystals by point-defect-mediated reversible domain switching. Nat. Mater. 3, 91 (2004).
B. Li, G. Li, Q. Yin, Z. Zhu, A. Ding, and W. Cao: Pinning and depinning mechanism of defect dipoles in PMN-PZT ceramics. J. Phys. D: Appl. Phys. 38, 1107 (2005).
A. Agronin, Y. Rosenwaks, and G. Rosenman: Direct observation of pinning centers in ferroelectrics. Appl. Phys. Lett. 88, 072911 (2006).
R. Schwartz, J. Voigt, B. Tuttle, D. Payne, T. Reichert, and R. DaSalla: Comments on the effects of solution precursor characteristics and thermal processing conditions on the crystallization behavior of sol-gel derived lead zirconate titanate thin films. J. Mater. Res. 12, 444 (1997).
J. Chang and S. Desu: Effects of dopants in PZT films. J. Mater. Res. 9, 955 (1994).
R.W. Whatmore, A. Patel, N. Shorrocks, and F.W. Ainger: Ferroelectric materials for thermal IR sensors state-of the-art and perspectives. Ferroelectrics 104, 269 (1990).
A. Bratkovsky and A. Levanyuk: Smearing of phase transition due to a surface or a bulk inhomogeneity in ferroelectric nanostructures. Phys. Rev. Lett. 94, 107601 (2005).
K. Brinkman, V. Cherman, D. Su, A. Tagantsev, and N. Setter: In-plane versus out-of-plane dielectric response in the thin-film relaxor Pb(Sc1/2Ta1/2)O3. Phys. Rev. B 73, 214112 (2006).
C. Stenger and A. Burggraaf: Order-disorder reactions in the ferroelectric perovskites Pb(Sc1/2Ta1/2)O3 and Pb(Sc1/2Nb1/2)O3 kinetics of the ordering process. Phys. Status Solidi 61, 275 (1980).
N. Setter and E. Cross: The role of B-site cation disorder in diffuse phase-transition behavior of perovskite ferroelectrics. J. Appl. Phys. 51, 4356 (1980).
K. Brinkman, A. Tagantsev, P. Muralt, and N. Setter: Self-polarization in Pb(Sc1/2Ta1/2)O3 thin films: Impact on dielectric and piezoelectric response. Jpn. J. Appl. Phys. 45,7288 (2006).
F. Chu: The ferroelectric phase transition in complex perkovskite relaxors. Ph.D. Thesis, Swiss Federal Institute of Technology EPFL, Lausanne, Switzerland (1994).
F. Chu, N. Setter, and A. Tagantsev: The spontaneous relaxor-ferroelectric transition of Pb(Sc1/2Ta1/2)O3. J. Appl. Phys. 74, 5129 (1993).
I. Reaney, D. Barber, and R. Watton: TEM studies of rf magnetron-sputtered thin films. J. Mater. Sci.-Mater. Electron. 3, 51 (1992).
R. Whatmore, Z. Huang, and M. Todd: Sputtered lead scandium tantalate thin films: Pb+4 in B sites in the perovskite structure. J. Appl. Phys. 82, 5686 (1997).
C. Bjormander, K. Sreenivas, A. Grishin, and K. Rao: Pyroelectric Pb(Sc0.5Ta0.5)O3/Y1Ba2Cu3O7−x thin film heterostructures. Appl. Phys. Lett. 67, 58 (1995).
Z. Huang, J. Battat, P. Donohue, M.A. Todd, and R.W. Whatmore: On the phase transformation kinetics in lead scandium tantalate thin films. J. Phys. D: Appl. Phys. 36, 3039 (2003).
R. Whatmore, A. Patel, and N. Shorrocks: Physicochemical properties of sol-gel derived lead scandium tantalate Pb(Sc0.5Ta0.5)O3 thin-films. Ferroelectrics 134, 343 (1992).
D. Liu and D. Payne: Lower temperature crystallization and ordering in sol-gel derived Pb(Sc0.5Ta0.5)O3 powders and thin layers. J. Appl. Phys. 77, 3361 (1995).
V. Fuflyigin, E. Salley, P. Vakhutinsky, A. Osinsky, J. Zhao, I. Gergis, and K. Whiteaker: Freestanding films of Pb(Sc0.5Ta0.5)O3 for uncooled infrared detectors. Appl. Phys. Lett. 78, 365 (2001).
N.A. Pertsev, A.G. Zembilgotov, and A.K. Tagantsev: Effect of mechanical boundary conditions on phase diagrams of epitaxial ferroelectric thin films. Phys. Rev. Lett. 80, 1988 (1998).
V. Nagarajan, S. Alpay, C. Ganpule, B. Nagaraj, S. Aggarwal, E. Williams, A. Roytburd, and R. Ramesh: Role of substrate on the dielectric and piezoelectric behavior of epitaxial lead magnesium niobate-lead titanate relaxor thin films. Appl. Phys. Lett. 77, 438 (2000).
G. Catalan, M. Corbett, R. Bowman, and J. Gregg: Effect of thermal expansion mismatch on the dielectric peak temperature of thin film relaxors. J. Appl. Phys. 91, 2295 (2002).
A. Seifert, N. Ledermann, S. Hiboux, J. Baborowski, P. Muralt, and N. Setter: Processing optimization of solution derived Pb(Zr1−xTix)O3 thin films for piezoelectric applications. Integrated Ferroelectrics 35, 1889 (2001).
P.K. Petrov, K. Sarma, and N.M. Alford: Evaluation of residual stress in thin ferroelectric films using grazing incident x-ray diffraction. Integrated Ferroelectrics 63, 695 (2004).
O. Vendik, S. Zubko, and M. Nikolski: Modeling and calculation of the capacitance of a planar capacitor containing a ferroelectric thin film. Tech. Phys. 44, 349 (1999).
S. Parola, R. Khem, D. Cornu, F. Chassagneux, S. Lecocq, Z. Kighelman, and N. Setter: Insights in the sol-gel processing of Pb(Mg1/3Nb2/3)O3. The synthesis and crown structure of a new lead magnesium cluster: Pb6Mg12(μ-OAc)6(μ2,n2-OAc)18(μ3, n2-OC2H4OPri)12. Inorg. Chem. Commun. 5, 316 (2002).
B. Malic, M. Kosec, I. Arcon, and A. Kodre: Homogeneity issues in chemical solution deposition of Pb(Zr,Ti)O3 thin films. J. Eur. Ceram. Soc. 25, 2241 (2005).
D. Liu, L. Ma, D. Payne, and D. Viehland: Sol-gel synthesis of Pb(Sc0.5Ta0.5)O3 powders and thin-layers. Mater. Lett. 17, 319 (1993).
B. Malic, I. Arcon, A. Kodre, and M. Kosec: EXAFS study of amorphous precursors for Pb(Zr,Ti)O3 ceramics. J. Sol.-Gel Sci. Technol. 16, 135 (1999).
B. Malic, M. Kosec, K. Smolej, and S. Stavber: Effect of precursor type on the microstructure of PbTiO3 thin films. J. Eur. Ceram. Soc. 19, 1345 (1999).
T. Boyle, D. Dimos, R. Schwartz, T. Alam, M. Sinclair, and C. Bucheit: Aging characteristics of a hybrid sol-gel Pb(Zr,Ti)O3 precursor solution. J. Mater. Res. 12, 1022 (1997).
A. Seifert, F. Lange, and J. Speck: Epitaxial-growth of PbTiO3 thin films on (001) SrTiO3 from solution precursors. J. Mater. Res. 10, 680 (1995).
P. Muralt, T. Maeder, L. Sagalowicz, S. Hiboux, S. Scalese, D. Naumovic, R. Agostino, N. Xanthopoulos, H. Mathieu, L. Patthey, and E. Bullock: Texture control of PbTiO3 and Pb(Zr,Ti)O3 thin films with TiO2 seeding. J. Appl. Phys. 83, 3835 (1998).
Z. Kighelman: Ph.D. Thesis. Swiss Federal Institute of Technology EPFL, Lausanne, Switzerland (2001).
T. Ostapchuk, J. Petzelt, V. Zelezny, A. Pashkin, J. Pokorny, I. Drbohlav, R. Kuzel, D. Rafaja, B. Gorshunov, M. Dressel, C. Ohly, S. Hoffman-Eifert, and R. Waser: Origin of soft-mode stiffening and reduced dielectric response in SrTiO3 thin films. Phys. Rev. B 66, 235406 (2002).
Author information
Authors and Affiliations
Corresponding author
Rights and permissions
About this article
Cite this article
Brinkman, K., Wang, Y., Cantoni, M. et al. Processing and properties of ferroelectric relaxor lead scandium tantalate Pb(Sc1/2Ta1/2)O3 thin films. Journal of Materials Research 22, 217–232 (2007). https://doi.org/10.1557/jmr.2007.0023
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1557/jmr.2007.0023