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Low-temperature ultraviolet sol-gel photoannealing processing of multifunctional lead-titanate-based thin films

Published online by Cambridge University Press:  31 January 2011

M.L. Calzada ,
I. Bretos ,
R. Jiménez ,
H. Guillon ,
J. Ricote  and
L. Pardo
M.L. Calzada*
Affiliation:
Instituto Ciencia de Materiales de Madrid (CSIC), Cantoblanco, 28049–Madrid, Spain
I. Bretos
Affiliation:
Instituto Ciencia de Materiales de Madrid (CSIC), Cantoblanco, 28049–Madrid, Spain
R. Jiménez
Affiliation:
Instituto Ciencia de Materiales de Madrid (CSIC), Cantoblanco, 28049–Madrid, Spain
H. Guillon
Affiliation:
KEMSTREAM, Advanced Vaporizers, Rue de la vieille poste, PIT de la Pompignane, Batiment T2, 34055 Montpellier, Cedex 1, France
J. Ricote
Affiliation:
Instituto Ciencia de Materiales de Madrid (CSIC), Cantoblanco, 28049–Madrid, Spain
L. Pardo
Affiliation:
Instituto Ciencia de Materiales de Madrid (CSIC), Cantoblanco, 28049–Madrid, Spain
*
a)Address all correspondence to this author. e-mail: lcalzada@icmm.csic.es
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Abstract

(Pb1−xCax)TiO3 perovskite thin films with nominal compositions of (Pb0.76Ca.24)TiO3 (ferroelectric) and (Pb0.50Ca0.50)TiO3 (relaxor-ferroelectric) were prepared on silicon substrates at low temperatures compatible with those used in Si-technology. The technique used for the processing of these films was ultraviolet (UV) sol-gel photoannealing, using photo-sensitive precursor solutions and UV-assisted rapid thermal processing. The UV-irradiation and thermal treatment of the solution-derived films (gel films) were carried out in air or in oxygen. In both cases, the formation of the perovskite occurred at the same temperature, and this temperature increased as the Ca2+ content increased. Thus, full-perovskite films of (Pb0.76Ca.24)TiO3 were obtained at 723 K whereas those of (Pb0.50Ca0.50)TiO3 were formed at 773 K. Well-defined ferroelectric hysteresis loops were measured in the (Pb0.76Ca.24)TiO3 films, with values of remanent polarization of Pr ∼ 11 μC cm−2 and coercive fields for the films processed in oxygen lower than those of the films processed in air, Ec ∼ 164 and ∼226 kV.cm−1, respectively. These films showed a ferro-paraelectric transition at close temperatures of Tmax ∼ 605 K, although with higher values of the permittivity for the film processed in oxygen, k ∼ 567 at 10 kHz. The (Pb0.50Ca.50)TiO3 films had a diffuse ferro-paraelectric transition with a relaxor-like character, also with higher k values for the films prepared in oxygen, k ∼ 179 at Tmax ∼ 20 K. The possible use of these materials in silicon integrated multifunctional devices is discussed in this paper.

Keywords

FilmPhotochemicalSol-gel
Type
Articles
Information
Journal of Materials Research , Volume 22 , Issue 7 , July 2007 , pp. 1824 - 1833
Copyright
Copyright © Materials Research Society 2007

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References

REFERENCES

1Schultz, M.: The end of the road for silicon? Nature 399, 729 1999CrossRefGoogle Scholar
2Semiconductor Industry Association: International Technology Roadmap for Semiconductors ITRS Edition 2005 available at http:/public.itrs.net/Common/2005ITRS/Home2005.htmGoogle Scholar
3Leong, M., Doris, B., Kedzierski, J., Rim, K. Yang, M.: Silicon device scaling to the sub-10-nm regime. Science 306, 2057 2004Google Scholar
4Boyd, I.W. Zhang, J.Y.: Photo-induced growth of dielectrics with excimer lamps. Solid-State Electron. 45, 1413 2001CrossRefGoogle Scholar
5Auciello, A., Scott, J.F. Ramesh, R.: The physics of ferroelectric memories. Phys. Today 51, 22 1998CrossRefGoogle Scholar
6Lakeman, C.D.E. Payne, D.A.: Processing effects in the sol-gel preparation of PZT dried gels, powders, and ferroelectric thin-layers. J. Am. Ceram. Soc. 75, 3091 1992CrossRefGoogle Scholar
7Wu, A., Vilarinho, P.M., Miranda-Salvado, I.M. Baptista, J.L.: Seeding studies in PZT thin films. Mater. Res. Bull. 33(1), 59 1998CrossRefGoogle Scholar
8Zhang, X.D., Meng, X.J., Sun, J.L., Liu, T. Chu, J.H.: Low-temperature preparation of highly (100)-oriented Pb(ZrxTi1−x)O3 thin film by high oxygen-pressure processing. Appl. Phys. Lett. 86, 252902 2005CrossRefGoogle Scholar
9Chang, S. Sivothaman, S.: Development of a low temperature MEMS process with a PECVD amorphous silicon structural layer. J. Micromech. Microeng. 16, 1307 2006CrossRefGoogle Scholar
10Van de Leest, R.E.: UV photo-annealing of thin sol-gel films. Appl. Surf. Sci. 86, 278 1995CrossRefGoogle Scholar
11Malic, B., Kosec, M., Arcon, I. Kodre, A.: Homogeneity issues in chemical solution deposition of Pb(Zr,Ti)O3 thin films. J. Eur. Ceram. Soc. 25, 2241 2005CrossRefGoogle Scholar
12Huang, A., Zhang, Q. Whatmore, R.W.: Low temperature crystallization of lead zirconate titanate thin films by a sol-gel method. J. Appl. Phys. 85, 7355 1999CrossRefGoogle Scholar
13Wu, A., Vilarinho, P.M., Reaney, I. Miranda Salvado, I.M.: Early stages of crystallization of sol-gel-derived lead zirconate titanate thin films. Chem. Mater. 15, 1147 2003CrossRefGoogle Scholar
14Li, Z.R., Wu, A. Vilarinho, P.M.: Perovskite phase stabilization of Pb(Zn1/3Ta2/3)O3 ceramics induced by PbTiO3 seeds. Chem. Mater. 16, 717 2004CrossRefGoogle Scholar
15Imai, H.: Handbook of Sol-Gel Science and Technology: Processing, Characterisation and Applications, edited by S. Sakka Kluwer Academic, Norwell, MA 2004 Vol. 1, Chap. 2, 639Google Scholar
16Calzada, M.L., Bretos, I., Jiménez, R., Guillon, H. Pardo, L.: Low-temperature processing of ferroelectric thin films compatible with silicon integrated circuit technology. Adv. Mater. 16, 1620 2004CrossRefGoogle Scholar
17Yu, J.J.: Formation of high-quality advanced high-k oxide layers at low temperature by excimer UV lamp-assisted photo-CVD and sol-gel processing. Chem. Res. Chinese U. 20, 396 2004Google Scholar
18Maekawa, S. Ohishi, T.: Evaluation of SiO2 thin-films prepared by sol-gel method using photoirradiation. J. Non-Cryst. Solids 169, 207 1994CrossRefGoogle Scholar
19Soyama, N., Sasaki, G., Atsuki, T., Yonezawa, T. Ogi, K.: Proceedings of the Ninth International Symposium on Applications of Ferroelectrics, ISAF’94 edited by R.K. Pandey, M. Liu, and A. Safari The Pennsylvania State University, NJ IEEE Catalog Number 94CH3416-5 1994 408Google Scholar
20Lim, T.Y., Yang, K.H., Kim, B.H. Auh, K.H.: Fabrication and characterization of direct patterning ferroelectric Sr0.9Bi2.1Ta2O9 thin films by photosensitive sol-gel solution. Thin Solid Films 471, 12 2005CrossRefGoogle Scholar
21Hayashi, T., Iizawa, N., Togawa, D., Yamada, M., Sakamoto, W., Kikuta, K. Hirano, S.I.: Excimer UV processing of (Bi,Nd)4Ti3O12 ferroelectric thin films by chemical solution deposition method. Jpn. J. Appl. Phys. 42, 5981 2003CrossRefGoogle Scholar
22Calzada, M.L., González, A., Poyato, R. Pardo, L.: Photo-sensitive sol-gel solutions for the low-temperature UV-assisted processing of PbTiO3 based ferroelectric thin films. J. Mater. Chem. 13, 1451 2003CrossRefGoogle Scholar
23Mendiola, J. Calzada, M.L.: Ferroelectric thin films of modified lead titanate in Handbook of Thin Film Materials edited by H. Nalwa Academic Press, London, UK 2002 Vol. 3, Chap. 6, 369Google Scholar
24Mendiola, J., Jiménez, R., Ramos, P., Bretos, I. Calzada, M.L.: Dielectric properties of Pb0.5Ca0.5TiO3 thin films. J. Appl. Phys. 98, 024106-1 2005CrossRefGoogle Scholar
25Chopra, S., Sharma, S., Goel, T.C. Mendiratta, R.G.: Ca substituted PbTiO3 thin films for infrared detectors. J. Electroceramics 13(1–3), 155 2004CrossRefGoogle Scholar
26Bretos, I., Ricote, J., Jiménez, R., Mendiola, J., Jiménez Rioboó, R.J. Calzada, M.L.: Crystallisation of Pb1−xCaTiO3 ferroelectric thin films as a function of the Ca2+ content. J. Eur. Ceram. Soc. 25, 2325 2005CrossRefGoogle Scholar
27Barnum, D.W.: Electronic absorption spectra of acetyl-acetonato complexes. 1. Complexes with trivalent transition metal ions. J. Inorg. Nucl. Chem. 21, 221 1961CrossRefGoogle Scholar
28Jiménez, R., Calzada, M.L. Mendiola, J.: Conditioning effects on RTP (Pb,Ca)TiO3 thin films. Thin Solid Films 335, 292 1998CrossRefGoogle Scholar
29Poyato, R., González, A., Calzada, M.L. Pardo, L.: High pyroelectric coefficients of Ca-modified lead titanate sol-gel thin films obtained by multiple deposition and crystallization. Ferroelectrics 271, 385 2002CrossRefGoogle Scholar
30Jiménez, R., Bretos, I., Ricote, J., Calzada, M.L. Mendiola, J.: Size effects on Pb0.5Ca0.5TiO3 thin films. J. Eur. Ceram. Soc. 25, 2319 2005CrossRefGoogle Scholar
31Zhang, Y., Terril, R.H. Bohn, P.W.: Ultraviolet photochemistry and ex situ ozonolysis of alkanethiol self-assembled monolayers on gold. Chem. Mater. 11, 2191 1999CrossRefGoogle Scholar