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Effects of the catalysts on the evolution of in-plane stress in alkoxide-derived silica gel coatings during heating

Published online by Cambridge University Press:  31 January 2011

Hiromitsu Kozuka  and
Tetsuya Iwase
Hiromitsu Kozuka*
Affiliation:
Department of Chemistry and Materials Engineering, Faculty of Chemistry, Materials and Bioengineering, Kansai University, Suita, Osaka-fu 564-8680, Japan
Tetsuya Iwase
Affiliation:
Department of Materials Science and Engineering, Faculty of Engineering, Kansai University, Suita, Osaka-fu 564-8680, Japan
*
a) Address all correspondence to this author. e-mail: [email protected]
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Abstract

The effects of the catalysts on the evolution of in-plane stress during heating were studied for silica gel coatings prepared from alkoxide solutions. Tetramethylorthosilicate was hydrolyzed in the presence of nitric acid, acetic acid, and ammonia as catalysts. Gel films were deposited on Si(100) wafers by spin coating, and heated at a constant rate of 5 °C/min up to 500 °C. During heating, in situ measurement of the in-plane stress was conducted by measuring the radius of curvature of the substrate. In-plane, tensile stress increased up to 560 and 370 MPa in the films prepared with HNO3 and CH3COOH, respectively. However, the stress was much smaller at 30–40 MPa, which remained almost constant during heating, for the films prepared with NH3. The much smaller stress resulted from the much lower degrees of the progress of densification during heating, which was revealed in the changes in thickness and infrared absorption spectra during heating. The low degrees of the progress of densification were caused by the colloidal nature of the gel films.

Keywords

CoatingSol-gelThin film
Type
Articles
Information
Journal of Materials Research , Volume 24 , Issue 8 , August 2009 , pp. 2511 - 2519
Copyright
Copyright © Materials Research Society 2009

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References

1Kozuka, H.: Stress evolution on gel-to-ceramic thin film conversion. J. Sol-Gel Sci. Technol. 40, 287 (2006).CrossRefGoogle Scholar
2Kozuka, H.: Fundamental issues on sol-gel coatings: Stress evolution, cracking and radiative striations, in Handbook of Sol-Gel Science and Technology: Processing, Characterization and Applications, Vol. 1, Sol-Gel Processing, edited by Sakka, S. (Kluwer Academic Publishers, Norwell, MA, 2005), p. 247.Google Scholar
3Rossetti, G.A. Jr., Cross, L.E., and Kushida, K.: Stress induced shift of the curie point in epitaxial PbTiO3 thin films. Appl. Phys. Lett. 59, 2524 (1991).CrossRefGoogle Scholar
4Hu, M.S., Thouless, M.D., and Evans, A.G.: The decohesion of thin-films from brittle substrates. Acta Metall. 36, 1301 (1988).CrossRefGoogle Scholar
5Cerqua, K.A., Hayden, J.E., and LaCourse, W.C.: Stress measurements in sol-gel films. J. Non-Cryst. Solids 100, 471 (1988).CrossRefGoogle Scholar
6Wu, W., Lanagan, M.T., Kullberg, M.L., Poeppel, R.B., Wang, B., and Danyluk, S.: The relationship between microstructure and re-sidual-stress in YBa2Cu3O7–x. Thin Solid Films 223, 260 (1993).CrossRefGoogle Scholar
7Syms, R.R.A. and Holmes, A.S.: Deposition of thick silica titania sol-gel films on Si substrates. J. Non-Cryst. Solids 170, 223 (1994).CrossRefGoogle Scholar
8Chingprado, E., Reynesfigueroa, A., Katiyar, R.S., Majumder, S.B., and Agrawal, D.C.: Raman-spectroscopy and x-ray-diffraction of PbTiO3 thin-film. J. Appl. Phys. 78, 1920 (1995).CrossRefGoogle Scholar
9Tuchiya, T., Itoh, T., Sasaki, G., and Suga, T.: Preparation and properties of piezoelectric lead zirconate titanate thin films for microsensors and microactuators by sol-gel processing. J. Ceram. Soc. Jpn. 104, 159 (1996).CrossRefGoogle Scholar
10Mehner, A., Klumper-Westkamp, H., Hoffmann, F., and Mayr, P.: Crystallization and residual stress formation of sol-gel-derived zirconia films. Thin Solid Films 308, 363 (1997).CrossRefGoogle Scholar
11Mendiola, J., Calzada, M.L., Ramos, P., Martin, M.J., and Agullo-Rueda, F.: On the effects of stresses in ferroelectric (Pb,Ca)TiO3 thin films. Thin Solid Films 315, 195 (1998).CrossRefGoogle Scholar
12Brenier, R. and Gagnaire, A.: Densification and aging of ZrO2 films prepared by sol-gel. Thin Solid Films 392, 142 (2001).CrossRefGoogle Scholar
13Brenier, R., Urlacher, C., Mugnier, J., and Brunel, M.: Stress development in amorphous zirconium oxide films prepared by sol-gel processing. Thin Solid Films 338, 136 (1999).CrossRefGoogle Scholar
14Zhang, L.L., Ichiki, M., and Maeda, R.: Stress measurements of Pt/PZT/Pt thin-film stack on oxidized silicon substrate for micro-actuator. Ferroelectrics 273, 2461 (2002).CrossRefGoogle Scholar
15Gupta, S.: Investigations of micro-stress and phase transition in sol-gel-derived multideposited coatings of barium titanate using Raman spectroscopy. J. Raman Spectrosc. 33, 42 (2002).CrossRefGoogle Scholar
16Hartner, W., Bosk, P., Schindler, G., Bachhofer, H., Mort, M., Wendt, H., Mikolajick, T., Dehm, C., Schroeder, H., and Waser, R.: SrBi2Ta2O9 ferroelectric thin film capacitors: Degradation in a hydrogen ambient. Appl. Phys. A 77, 571 (2003).CrossRefGoogle Scholar
17Robertson, M.A., Rudkin, R.A., Parsonage, D., and Atkinson, A.: Mechanical and thermal properties of organic/inorganic hybrid coatings. J. Sol-Gel Sci. Technol. 26, 291 (2003).Google Scholar
18Exarhos, G.J. and Hess, N.J.: Spectroscopic measurements of stress-relaxation during thermally induced crystallization of amorphous titania films. Thin Solid Films 220, 254 (1992).CrossRefGoogle Scholar
19Parrill, T.M.: Heat-treatment of spun-on acid-catalyzed sol-gel silica films. J. Mater. Res. 9, 723 (1994).CrossRefGoogle Scholar
20Sengupta, S.S., Park, S.M., Payne, D.A., and Allen, L.H.: Origins and evolution of stress development in sol-gel derived thin layers and multideposited coatings of lead titanate. J. Appl. Phys. 83, 2291 (1998).CrossRefGoogle Scholar
21Chow, L.A., Dunn, B., Tu, K.N., and Chiang, C.: Mechanical properties of xerogel silica films derived from stress versus temperature and cracking experiments. J. Appl. Phys. 87, 7788 (2000).CrossRefGoogle Scholar
22Chiang, C.K., Wallace, W.E., Lynn, G.W., Feiler, D., and Xia, W.: Thermally induced stress relaxation and densification of spin-on-glass thin films. Appl. Phys. Lett. 76, 430 (2000).CrossRefGoogle Scholar
23Pulskamp, J.S., Wickenden, A., Polcawich, R., Piekarski, B., Dubey, M., and Smith, G.: Mitigation of residual film stress deformation in multilayer microelectromechanical systems cantilever devices. J. Vac. Sci. Technol., B 21, 2482 (2003).CrossRefGoogle Scholar
24Kurisu, T. and Kozuka, H.: Effects of the heating rate on stress evolution in alkoxide-derived silica gel coating films. J. Am. Ceram. Soc. 89, 2453 (2006).CrossRefGoogle Scholar
25Kozuka, H. and Komeda, M.: Effect of the amount of water for hydrolysis on cracking and stress evolution in alkoxide-derived sol-gel silica coating films. J. Ceram. Soc. Jpn. 112, S223 (2004).Google Scholar
26Kozuka, H., Miyake, H., and Ishikawa, Y.: Cracking and stress evolution in alkoxide-derived gel coating films on firing, in XX International Congress on Glass Proceedings (CD-ROM), edited by Yoko, T. (The Ceramic Society of Japan, Tokyo, 2004), paper O–11.Google Scholar
27Ishikawa, Y. and Kozuka, H.: Evolution of stress in alkoxide-derived titania gel films under heat-treatment: Effects of polyvi-nylpyrrolidone and acetic acid in coating solutions. J. Ceram. Soc. Jpn. 112, S228 (2004).Google Scholar
28Brinker, C.J. and Scherer, G.W.: Sol-Gel Science: The Physics and Chemistry of Sol-Gel Processing (Academic Press, Boston, 1990), Chap. 2.Google Scholar
29Hoffman, R.W.: The mechanical properties of thin condensed films, in Physics of Thin Films, Vol. 3, edited by Hass, G., Francombe, M.H., Hoffman, R.W., and Vossen, J.L. (Academic Press, New York, 1966), p. 211.Google Scholar
30Brantley, W.A.: Calculated elastic constants for stress problems associated with semiconductor devices. J. Appl. Phys. 44, 534 (1973).CrossRefGoogle Scholar
31Riter, E.: Dielectric film materials for optical applications, in Physics of Thin Films, Vol. 8, edited by Hass, G., Francombe, M.H., and Hoffmann, R.W. (Academic Press, New York, 1975), p. 1.Google Scholar
32Yahata, R. and Kozuka, H.: Stress evolution of sol-gel-derived silica coatings during heating: The effects of the chain length of alcohols as solvents. Thin Solid Films 517, 1983 (2009).CrossRefGoogle Scholar
33Brinker, C.J. and Scherer, G.W.: Sol-Gel Science: The Physics and Chemistry of Sol-Gel Processing (Academic Press, Boston, 1990), Chap. 9, Sec. 2.2.2.Google Scholar
34Kingery, W.D., Bowen, H.K., and Uhlmann, D.R.: Introduction to Ceramics, 2nd Ed. (John Wiley & Sons, New York, 1976), Chap. 16.Google Scholar