Hostname: page-component-5c6d5d7d68-ckgrl Total loading time: 0 Render date: 2024-08-06T12:13:30.118Z Has data issue: false hasContentIssue false

Dielectric and microstructural properties of barium titanate zirconate thin films on copper substrates

Published online by Cambridge University Press:  03 March 2011

J.F. Ihlefeld*
Affiliation:
North Carolina State University, Department of Materials Science and Engineering, Raleigh, North Carolina 27695
J-P. Maria
Affiliation:
North Carolina State University, Department of Materials Science and Engineering, Raleigh, North Carolina 27695
W. Borland
Affiliation:
DuPont Electronic Technologies, Research Triangle Park, North Carolina 27709
*
a)Address all correspondence to this author. e-mail: jfihlefe@unity.ncsu.edu
Get access

Abstract

Barium titanate zirconate, Ba(Ti1−xZrx)O3 (0 ≤ x ≤ 0.25), thin films were deposited via the chemical solution deposition (CSD) method directly on copper foils. The films were processed in a reductive atmosphere containing nitrogen, water vapor, and hydrogen gas at 900 °C to preserve the metallic copper substrate during crystallization. Increasing the fraction of BaZrO3 revealed several effects, including an increase in unit cell dimensions, a decrease in both the temperature and value of the maximum permittivity, as well as a decrease in the average grain size of the films. The decrease in the relative permittivity was attributed to a grain size effect as opposed to zirconium substitution. In film compositions containing 25 mol% BaZrO3, the permittivity below Tmax became dispersive, and the ferroelectric transitions became increasingly diffuse. These characteristics suggest relaxor-like behavior. The dielectric tunability of Ba(Ti1−xZrx)O3 was studied at room temperature and at Tmax for each composition. There was little variation in the tunability with measurement temperature; however compositions that were ferroelectric at room temperature saw a decrease in hysteresis at Tmax, and all compositions showed an increase in permittivity.

Type
Articles
Copyright
Copyright © Materials Research Society 2005

Access options

Get access to the full version of this content by using one of the access options below. (Log in options will check for institutional or personal access. Content may require purchase if you do not have access.)

References

REFERENCES

1Hofer, C., Hoffmann, M., Boettger, U. and Waser, R.: Relaxors as high -ε- materials for multilayer and thin film capacitors. Ferroelectrics 270, 179 (2002).CrossRefGoogle Scholar
2Mizuno, Y., Morita, K., Hagiwara, T., Kishi, H., Ohnuma, K. and Ohsato, H.: Relationship between microstructural evolution and electrical properties in Ba(Ti,Zr)O3-based materials for Ni-MLCC. Jpn. J. Appl. Phys. 43, 6640 (2004).CrossRefGoogle Scholar
3Neirman, S.M.: The Curie point temperature of Ba(Ti1−xZrx)O3 solid solutions. J. Mater. Sci. 23, 3973 (1988).CrossRefGoogle Scholar
4Jonker, G.H.: Capacitor materials with high-dielectric constant. Philips Technical Review 17(5), 129 (1955).Google Scholar
5Verbitskaia, T.N., Zhdanov, G.S., Venevtsev, I.N. and Soloviev, S.P.: Electrical and x-ray diffraction studies of the BaTiO3–BaZrO3 system. Sov. Phys. Crystallogr. 3, 182 (1958).Google Scholar
6Cross, L.E.: Relaxor ferroelectrics: An overview. Ferroelectrics 151, 302 (1994).CrossRefGoogle Scholar
7Tang, X.G., Chew, K-H. and Chan, H.L.W.: Diffuse phase transition and dielectric tunability of Ba(ZryTi1−y)O3 relaxor ferroelectric ceramics. Acta Mater. 52, 5177 (2004).CrossRefGoogle Scholar
8Wada, S., Adachi, H., Kakemoto, H., Chazono, H., Mizuno, Y., Kishi, H. and Tsurumi, T.: Phase transition behaviors of BaTiO3–BaZrO3 solid solutions under high direct current bias fields. J. Mater. Res. 17, 456 (2002).CrossRefGoogle Scholar
9Ravez, J. and Simon, A.: Temperature and frequency dielectric response of ferroelectric ceramics with composition Ba(Ti1−xZrx)O3. Eur. J. Solid State Inorg. Chem. 34, 1199 (1997).Google Scholar
10Dixit, A., Majumder, S.B., Dobal, P.S., Katiyar, R.S. and Bhalla, A.S.: Phase transition studies of sol-gel deposited barium zirconate titanate thin films. Thin Solid Films 447–448, 284 (2004).CrossRefGoogle Scholar
11Tohma, T., Masumoto, H. and Goto, T.: Dielectric properties of Ba(Ti0.85Zr0.15)O3 films prepared by metalorganic chemical vapor deposition. Jpn. J. Appl. Phys. 42, 6969 (2003).CrossRefGoogle Scholar
12Tanaka, K., Suzuki, K., Fu, D., Nishizawa, K., Miki, T. and Kato, K.: Grain size effect on dielectric and piezoelectric properties of alkoxy-derived BaTiO3-based thin films. Jpn. J. Appl. Phys. 43, 6525 (2004).CrossRefGoogle Scholar
13Dawley, J.T., Ong, R.J. and Clem, P.G.: Chemical solution deposition of 〈100〉-oriented SrTiO3 buffer layers on Ni substrates. J. Mater. Res. 17, 1678 (2002).CrossRefGoogle Scholar
14Ong, R.J., Dawley, J.T. and Clem, P.G.: Chemical solution deposition of biaxially oriented (Ba,Sr)TiO3 thin films on 〈100〉 Ni. J. Mater. Res. 18, 2310 (2003).CrossRefGoogle Scholar
15Ihlefeld, J., Laughlin, B., Hunt-Lowery, A., Borland, W., Kingon, A. and Maria, J-P.: Copper compatible barium titanate thin films for embedded passives. J. Electroceram. 14(2), 95 (2005).CrossRefGoogle Scholar
16Laughlin, B.J., Ihlefeld, J.F. and Maria, J-P.: Preparation of sputtered (BaxSr1−x)TiO3 thin films directly on copper. J. Am. Ceram. Soc. 2005 , (in press).CrossRefGoogle Scholar
17Losego, M.D., Jimison, L.H., Ihlefeld, J.F. and Maria, J-P. Ferroelectric response of lead zirconate titanate thin films prepared directly on low resistivity copper substrates. Appl. Phys. Lett. 86, 172906 (2005).CrossRefGoogle Scholar
18Maria, J-P., Cheek, K., Streiffer, S., Kim, S-H., Dunn, G. and Kingon, A.: Lead zirconate titanate thin films on base-metal foils: An approach for embedded high K passive components. J. Amer. Cer. Soc. 84, 2436 (2001).CrossRefGoogle Scholar
19Zou, Q., Ruda, H.E., Yacobi, B.G., Saegusa, K. and Farrell, M.: Improved dielectric properties of lead zirconate titanate thin films deposited on metal foils with LaNiO3 buffer layers. Appl. Phys. Lett. 78, 1282 (2001).CrossRefGoogle Scholar
20Kim, D.J., Kaufman, D.Y., Streiffer, S.K., Lee, T.H., Erck, R., and Auciello, O.: Chemical solution deposition of PLZT thin films on base metal foils, in Ferroelectric Thin Films XI, edited by Kaufman, D.Y., Hoffmann-Eifert, S., Gilbert, S.R., Aggarwal, A., and Shimizu, M. (Mater. Res. Soc. Symp. Proc. 748, Warrendale, PA, 2003), p. 457.Google Scholar
21Kim, T., Kingon, A.I., Maria, J-P. and Croswell, R.T.: Ca-doped lead zirconate titanate thin film capacitors on bas metal nickel on copper foil. J. Mater. Res. 19, 2841 (2004).CrossRefGoogle Scholar
22Siegal, M.P., Clem, P.G., Dawley, J.T., Ong, R.J., Rodriguez, M.A. and Overmyer, D.L.: All solution-chemistry approach for YBa2Cu3O7−δ-coated conductors. Appl. Phys. Lett. 80, 2710 (2002).CrossRefGoogle Scholar
23Cullity, B.D. and Stock, S.R.: Elements of X-Ray Diffraction, 3rd ed. (Prentice Hall, Upper Saddle River, NJ, 2001), p. 366.Google Scholar
24Data, International Centre for Diffraction Swarthmore, PA, 1988.Google Scholar
25Arlt, G., Hennings, D. and de With, G.: Dielectric-properties of fine-grained barium-titanate ceramics. J. Appl. Phys. 58, 1619 (1985).CrossRefGoogle Scholar
26Parker, C.B., Maria, J-P. and Kingon, A.I.: Temperature and thickness dependent permittivity of (Ba,Sr)TiO3 thin films. Appl. Phys. Lett. 81, 340 (2002).CrossRefGoogle Scholar
27Frey, M.H., Xu, Z., Han, P. and Payne, D.A.: The role of interfaces on an apparent grain size effect on the dielectric properties for ferroelectric barium titanate ceramics. Ferroelectrics 206–207, 937 (1998).Google Scholar
28Polotai, A.V., Ragula, A.V. and Randall, C.A.: Preparation and size effect in pure nanocrystalline barium titanate ceramics. Ferroelectrics 288, 93 (2003).CrossRefGoogle Scholar
29Wada, S., Yasuno, H., Hoshina, T., Nam, S-M., Kakemoto, H. and Tsurumi, T.: Preparation of nm-sized barium titanate fine particles and their powder dielectric properties. Jpn. J. Appl. Phys. 41, 6188 (2003).CrossRefGoogle Scholar
30Tang, X.G., Wang, J., Wang, X.X. and Chan, H.L.W.: Effects of grain size on the dielectric properties and tunabilities of sol-gel derived Ba(Zr0.2Ti0.8)O3 ceramics. Solid State Commun. 131, 163 (2004).CrossRefGoogle Scholar
31Kell, R.C. and Hellicar, N.J.: Structural transitions in barium titanate-zirconate transducer materials. Acoustica 6, 235 (1956).Google Scholar