Hostname: page-component-78c5997874-g7gxr Total loading time: 0 Render date: 2024-11-05T16:26:17.415Z Has data issue: false hasContentIssue false
  • English
  • Français

Composition and chemical width of ultrathin amorphous films at grain boundaries in silicon nitride

Published online by Cambridge University Press:  31 January 2011

H. Gu ,
R. M. Cannon  and
M. Rühle
H. Gu
Affiliation:
Japan Science and Technology Corporation, “Ceramics Superplasticity” project, JFCC 2F, 2-4-1 Mutsuno, Atusta, Nagoya 456, Japan and Max-Planck-Institut für Metallforschung, Seestraβe 92, 70174, Stuttgart, Germany
R. M. Cannon
Affiliation:
Lawrence Berkeley Laboratory, University of California, Berkeley, California 94720
M. Rühle
Affiliation:
Max-Planck-Institut für Metallforschung, Seestraβe 92, 70174, Stuttgart, Germany
Get access

Extract

Two different electron energy loss spectroscopy (EELS) quantitative analytical methods for obtaining complete compositions from interface regions are applied to ultrathin oxide-based amorphous grain boundary (GB) films of ∼ 1 nm thickness in high-purity HIPed Si3N4 ceramics. The first method, 1, is a quantification of the segregation excess at interfaces for all the elements, including the bulk constituents such as silicon and nitrogen; this yields a GB film composition of SiN0.49±1.4O1.02±0.42 when combined with the average film thickness from high resolution electron microscopy (HREM). The second method, II, is based on an EELS near-edge structure (ELNES) analysis of the Si–L2,3 edge of thin GB films which permits a subtraction procedure that yields a completeEELS spectrum, e.g., that also includes the O–K and N–K edges, explicitly for the GB film. From analysis of these spectra, the film composition is directly obtained as SiN0.63±0.19O1.44±0.33, close to the one obtained by the first method but with much better statistical quality. The improved quality results from the fewer assumptions made in method II; while in method I uniform thickness and illumination condition have to beassumed, and correction of such effects yields an extra systematic error. Method II is convenient as it does not depend on the film thickness detected by HREM, nor suffer from material lost by preferential thinning at the GB. In addition, a chemical width for these films can be deduced as 1.33 ± 0.25 nm, that depends on an estimation of film density based on its composition. Such a chemical width is in good agreement with the structural thickness determined by HREM, with a small difference that is probably due to the different way in which these techniques probe the GB film. The GB film compositions are both nonstoichiometric, but in an opposite sense, this discrepancy is probably due to different ways of treating the surface oxidation layers in both methods.

Type
Articles
Information
Journal of Materials Research , Volume 13 , Issue 2 , February 1998 , pp. 376 - 387
Copyright
Copyright © Materials Research Society 1998

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.Clarke, D.R., Ultramicroscopy 4, 33 (1979).CrossRefGoogle Scholar
2.Tsai, R. L. and Raj, R., J. Am. Ceram. Soc. 63, 513 (1980).CrossRefGoogle Scholar
3.Raj, R., J. Geophys. Rev. B 87, 4731 (1982).CrossRefGoogle Scholar
4.Lange, F. F., Am. Ceram. Soc. Bull. 62, 1368 (1983).Google Scholar
5.Cinibulk, M.K., Kleebe, H-J., and Rühle, M., J. Am. Ceram. Soc. 76, 426 (1993).CrossRefGoogle Scholar
6.Kleebe, H-J., Cinibulk, M.K., Cannon, R.M., and Rühle, M., J. Am. Ceram. Soc. 76, 1969 (1993).CrossRefGoogle Scholar
7.Clarke, D.R., Ultramicroscopy 4, 33 (1979).CrossRefGoogle Scholar
8.Clarke, D.R., Shaw, T.M., Philips, A. P., and Horn, R.G., J. Am. Ceram. Soc. 76, 1201 (1993).CrossRefGoogle Scholar
9.Kleebe, H-J., Hoffmann, M. J., and Rühle, M., Z. Metalld. 83, 610 (1992).Google Scholar
10.Tanaka, I., Kleebe, H-J., Cinibulk, M.K., Bruley, J., Clarke, D.R., and Rühle, M., J. Am. Ceram. Soc. 77, 911 (1994).CrossRefGoogle Scholar
11.Clarke, D.R., in Tailoring of Mechanical Properties of Si3N4 Ceramics, edited by Hoffmann, M. J. and Petzow, G. (NATO ASI Series E: Applied Sciences 276, Kluwer Academic Publishers, Dordrecht, The Netherlands, 1994), p. 291.CrossRefGoogle Scholar
12.Ikeda, J.A. S., Chiang, Y-M., Garratt-Reed, A. J., and Vander Sande, J. B., J. Am. Ceram. Soc. 76, 2447 (1993).CrossRefGoogle Scholar
13.Chiang, Y-M., Silverman, L.A., French, R.H., and Cannon, R.M., J. Am. Ceram. Soc. 77, 1143 (1994).CrossRefGoogle Scholar
14.Bruley, J., Tanaka, I., Kleebe, H-J., and Rühle, M., Anal. Chim. Act. 297, 97 (1994).CrossRefGoogle Scholar
15.Gu, H., Pan, X., Cannon, R.M., and Rühle, M., J. Am. Ceram. Soc. (to be published).Google Scholar
16.Bruley, J., Ultramicroscopy 4, 33 (1979).Google Scholar
17.Gu, H., Ceh, M., Stemmer, S., Müllejans, H., and Rühle, M., Ultramicroscopy 59, 215 (1995).CrossRefGoogle Scholar
18.Tanaka, I., Pezzotti, G., Okamoto, T., and Mitamoto, Y., J. Am. Ceram. Soc. 72, 1656 (1989).CrossRefGoogle Scholar
19.Egerton, R., Electron Energy-Loss Spectroscopy in Electron Mi-croscopes (Plenum Press, New York and London, 1996).CrossRefGoogle Scholar
20.Shuman, H. and Somlyo, A. P., Ultramicroscopy 21, 23 (1987).CrossRefGoogle Scholar
21.Leapman, R.D. and Swyt, C. R., Ultramicroscopy 26, 393 (1988).CrossRefGoogle Scholar
22.Tencé, M., Quartuccio, M., and Colliex, C., Ultramicroscopy 58, 42 (1995).CrossRefGoogle Scholar
23.Tanaka, I., Bruley, J., Gu, H., Hoffmann, M. J., Kleebe, H-J., Cannon, R.M., Clarke, D.R., and Rühle, M., in Tailoring of Mechanical Properties of Si3N4 Ceramics, edited by Hoffmann, M. J. and Petzow, G. (NATO ASI Series E: Applied Sciences 276, Kluwer Academic Publishers, Dordrecht, The Netherlands, 1994), p. 275.CrossRefGoogle Scholar