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Aging Characteristics of a Hybrid Sol-gel Pb(Zr, Ti)O3 Precursor Solution

Published online by Cambridge University Press:  31 January 2011

Timothy J. Boyle ,
Duane Dimos ,
Robert W. Schwartz ,
Todd M. Alam ,
Michael B. Sinclair  and
Catherine D. Buchheit
Timothy J. Boyle*
Affiliation:
Advanced Materials Laboratory, Sandia National Laboratories, 1001 University Boulevard, SE, Albuquerque, New Mexico 87106
Duane Dimos
Affiliation:
Sandia National Laboratories, 1515 Eubank NE, Mail Stop 1405, Albuquerque, New Mexico 87715
Robert W. Schwartz
Affiliation:
Advanced Materials Laboratory, Sandia National Laboratories, 1001 University Boulevard, SE, Albuquerque, New Mexico 87106
Todd M. Alam
Affiliation:
Sandia National Laboratories, 1515 Eubank NE, Mail Stop 1405, Albuquerque, New Mexico 87115
Michael B. Sinclair
Affiliation:
Sandia National Laboratories, 1515 Eubank NE, Mail Stop 1405, Albuquerque, New Mexico 87115
Catherine D. Buchheit
Affiliation:
Advanced Materials Laboratory, Sandia National Laboratories, 1001 University Boulevard, SE, Albuquerque, New Mexico 87106
*
a)Author to whom correspondence should be addressed.
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Abstract

The “aging” characteristics of an acetic acid/methanol solvent-based lead zirconate titanate (PZT) precursor solution, prepared by the Inverted Mixing Order (IMO) process, have been studied for an extended period of time. The changes in film properties were characterized using optical microscopy, optical scattering, and ferroelectric testing. Films generated from the IMO process exhibit an increase in thickness as a function of solution age due to chemical “aging” (esterification) of the precursor solution. This increased thickness results in a decrease in the microstructural uniformity, which affects the electrical and optical properties. In order to understand and eventually control this phenomenon, we have quantified the “aging” of this solution using a variety of analytical methods, including 1H NMR spectroscopy, pH measurements, and Fourier transform infrared (FTIR) spectroscopy. It is of note that we have discovered a method that circumvents this “aging” problem by removal of the volatile material, forming an IMO powder which can be redissolved to produce high quality PZT thin films whenever desired.

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Type
Articles
Information
Journal of Materials Research , Volume 12 , Issue 4 , April 1997 , pp. 1022 - 1030
Copyright
Copyright © Materials Research Society 1997

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References

1.Wi, G., Wu, Z., and Sayer, M., J. Appl. Phys. 64, 2717 (1988).Google Scholar
2.Budd, K. D., Dey, S. K., and Payne, D. A., Brit. Ceram. Soc. Proc. 36, 107 (1985).Google Scholar
3.Fukushima, J., Kodaira, K., and Marsushita, T., J. Mater. Sci. 19, 595 (1984).CrossRefGoogle Scholar
4.Haertling, G. H., Ferroelectrics 116, 51 (1991).CrossRefGoogle Scholar
5.Schwartz, R. W., Assink, R. A., and Headley, T. J., in Ferroelectric Thin Films II, edited by Kingon, A. I., Myers, E. R., and Tuttle, B. (Mater. Res. Soc. Symp. Proc. 243, Pittsburgh, PA, 1992), p. 245.Google Scholar
6.Vest, R. W. and Xu, J., Ferroelectrics 93, 21 (1989).CrossRefGoogle Scholar
7.Assink, R. A. and Schwartz, R. W., Chem. Mater. 5, 511 (1993).CrossRefGoogle Scholar
8.Tuttle, B. A. and Schwartz, R. W., Mater. Res. Soc. Bull. 21, 49 (1996).CrossRefGoogle Scholar
9.Boyle, T. J., Alam, T. M., Warren, W. L., Rosay, M. M., and Buchheit, C. D., unpublished.Google Scholar
10.Doeuff, S., Dromzee, Y., Taullele, F., and Sanchez, C., Inorg. Chem. 28, 4439 (1989).CrossRefGoogle Scholar
11.Prabakar, S., Assink, R. A., Raman, N. K., and Brinker, C. J., in Better Ceramics Through Chemistry VI, edited by Cheetham, A. K., Brinker, C. J., Mecartney, M. L., and Sanchez, C. (Mater. Res. Soc. Symp. Proc. 346, Pittsburgh, PA, 1994), p. 979.Google Scholar
12.Boyle, T. J., Schwartz, R. W., Doedens, R. J., and Ziller, J. W., Inorg. Chem. 34, 1110 (1995).CrossRefGoogle Scholar
13.Sinclair, M., Dimos, D., Potter, B. G., Schwartz, R. W., and Buchheit, C. D., Int. Ferroelectrics 11, 25 (1995).CrossRefGoogle Scholar
14.Potter, B. G., Sinclair, M. B., and Dimos, D., Appl. Phys. Lett. 63, 2180 (1993).CrossRefGoogle Scholar
15.Sinclair, M. B., Dimos, D. B., Potter, B. G., and Schwartz, R. W., J. Am. Ceram. Soc. 78, 2027 (1995).CrossRefGoogle Scholar
16.Schwartz, R. W., Voigt, J. A., Tuttle, B. A., Payne, D. A., Reichert, T. L., and DaSalla, R. S., J. Mater. Res. 12, 444 (1997).CrossRefGoogle Scholar
17.Lefevre, M. J., Speck, J. S., Schwartz, R. W., Dimos, D., and Lockwood, S. J., J. Mater. Res. 11, 2076 (1996).CrossRefGoogle Scholar
18. A crystal of {[Pb(O2CMe)2·py]2}∞ was isolated from an IMO mixture which had pyridine added to aid in crystallization. {[Pb(O2CMe)2·py]2}∞ was solved in the P21/n space group with a = 9.039 (1) Å, b = 10.196 (1), c = 24.970 (2), °, and V = 2272(1) Å3 for Z = 4. Full details will be reported shortly. The ease of crystallization and high yield implies that the Pb component of the IMO was not intimately mixed with the Ti/Zr alkoxides.Google Scholar
19.Day, V. W., Eberspacher, T. A., Chen, Y., Hao, J., and Klemperer, W. G., Inorganica Chim. Acta 229, 391 (1995).CrossRefGoogle Scholar
20. Final film properties and precursor structures have been found to be influenced by ester formation. Lakeman, C. D. E., M. S.Thesis, University of Illinois (1991).Google Scholar
21.Masterton, W. L. and Slowinski, E. J., Chemical Principles (W. B. Saunders Co., Philadelphia PA, 1977), pp. 448–450.Google Scholar
22. A patent application (Sandia reference number SD-5548) has been filed on this technique.Google Scholar
23.Bradley, D. C., Mehrotra, R. C., and Gaur, D. P., Metal Alkoxides (Academic Press, New York, 1978), pp. 117–122.Google Scholar
24. Personal communication with S. J. Lockwood of Sandia National Laboratories.Google Scholar
25.Toyoda, M., Hamaji, Y., Tomono, K., and Payne, D. A., Jpn. J. Appl. Phys., Part I 32, 4158 (1993).CrossRefGoogle Scholar