Hostname: page-component-586b7cd67f-2brh9 Total loading time: 0 Render date: 2024-11-25T02:26:34.713Z Has data issue: false hasContentIssue false

Low-Temperature Processing of Sol-Gel Derived Metal Oxide Thin Films using Supercritical Carbon Dioxide Fluid

Published online by Cambridge University Press:  15 March 2011

Hiroshi Uchida
Affiliation:
Department of Materials and Life Sciences, Faculty of Science and Technology, Sophia University, 7-1 Kioi-cho, Chiyoda-ku, Tokyo, 102-8554, Japan
Kaori Fujioka
Affiliation:
Department of Materials and Life Sciences, Faculty of Science and Technology, Sophia University, 7-1 Kioi-cho, Chiyoda-ku, Tokyo, 102-8554, Japan
Seiichiro Koda
Affiliation:
Department of Materials and Life Sciences, Faculty of Science and Technology, Sophia University, 7-1 Kioi-cho, Chiyoda-ku, Tokyo, 102-8554, Japan
Get access

Abstract

We demonstrate a novel technique using supercritical carbon dioxide (scCO2) fluid for lowering processing temperature of sol-gel-derived metal oxide thin films. The film processing was performed in a hot-wall closed vessel filled with scCO2 fluid. The effects of fluid temperature and additives on the sol-gel synthesis reaction under scCO2 fluid were also investigated. Precursor films of titanium dioxide (TiO2) prepared on silicon wafer and silica glass by sol-gel coating using Ti-alkoxide were converted to crystalline TiO2 (anatase) films successfully by treatment in scCO2 without additive agent at a fluid pressure of 15 MPa and at a substrate temperature of above 250°C, which is significantly lower than the processing temperature of conventional sol-gel deposition. Furthermore, additive agents such as water (H2O) and nitrogen-oxygen mixture (N2-O2) promoted the decomposition and crystallization of precursor films in scCO2 fluid to form the crystalline TiO2 (anatase) films at a substrate temperature at as low as 200°C although it also produced surface absorbates consisted of hydroxides on the film surface. The experimental results suggested that the hydrolysis and polymerization reactions of Ti-alkoxide in the precursor films were proceeded by the scCO2 processing to form titanium-oxygen (Ti-O) networks and that byproducts such as alcohols were removed from the resulting films.

Type
Research Article
Copyright
Copyright © Materials Research Society 2009

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

1. Tohge, N., Shinmou, K. and Minami, T.: J. Sol-Gel Sci. Technol. 2 (1994) 581.Google Scholar
2. Leest, R. E. Van de: Appl. Surf. Sci. 86 (1995) 278.Google Scholar
3. Taylor, D. J. and Fabes, B. D.: J. Non-Cryst. Solids 147–148 (1992) 457.Google Scholar
4. Levine, T. E., Keddie, J. L., Revesz, P., Mayer, J. W. and Giannelis, E. P.: J. Am. Ceram. Soc. 76 (1993) 1369.Google Scholar
5. Yoda, S., Otaka, K., Takebayashi, Y., Sugeta, T. and Sato, T.: J. Non-Cryst. Solids 285 (2001) 8.Google Scholar
6. Stallings, W. E. and Lamb, H. H.: Langmuir 19 (2003) 2989.Google Scholar
7. Wakayama, H., Goto, Y. and Fukushima, Y.: Phys. Chem. Chem. Phys. 5 (2003) 3784.Google Scholar
8. Jessop, P. G., Ikariya, T. and Noyori, R.: Science 269 (1995) 1065.Google Scholar
9. Woods, R. J. and Busby, D. C.: Mater. Perfom. 34 (10095) No. 11, 45.Google Scholar
10. Sako, T.: Supercritical Fluids, eds. Arai, Y., Sako, T. and Takebayashi, Y. (Springer, Berlin, 2002) p. 357.Google Scholar
11. Shimomura, K., Tsurumi, T., Ohba, Y. and Daimon, M.: Jpn. J. Appl. Phys. 30 (1991) 2174.Google Scholar
12. Cheng, H., Ma, J., Zhao, Z. and Qi, L.: Chem. Mater. 7 (1995) 663.Google Scholar
13. Somiya, S. and Roy, R.: Bull. Mater. Sci. 23 (2000) 453.Google Scholar
14. Morita, T., Wagatsuma, Y., Cho, Y., Morioka, H., Funakubo, H., and Setter, N.: Appl. Phys. Lett. 84 (2004) 5094.Google Scholar
15. Ryu, H. K., Heo, J. S., Cho, S. I. and Moon, S. H.: J. Electrochem. Soc. 146 (1999) 1117.Google Scholar
16. Bessergenev, V. G.., Khmelinskii, I. V., Pereira, R. J. F., Krisuk, V. V., Turgambaeva, A. E. and Igumenov, I. K.: Vacuum 64 (2002) 275.Google Scholar
17. Urlaub, R., Posset, U. and Thull, R.: J. Non-Cryst. Solids 265 (2000) 276.Google Scholar
18. Fujii, H., Inata, K., Ohtaki, M., Eguchi, K. and Arai, H., J. Mater. Sci. 36 (2001) 527.Google Scholar
19. Terabe, K., Kato, K., Miyazaki, H., Yamaguchi, S., Imai, A. and Iguchi, Y.: J. Mater. Sci. 29(1994) 1617.Google Scholar
20. Wang, W., Gu, B., Liang, L., Hamilton, W. A. and Wesolowski, D. J.: J. Phys. Chem. B 108, (2004) 14789.Google Scholar
21. Hu, Y. and Yuan, C.: J. Cryst. Growth 274274274 274 (2005) 563.Google Scholar