Si₃N₄ and Ge₃N₄ belong to a family of nonoxide ceramics. They exhibit unique physico-chemical and mechanical properties making them suitable for various applications. Si₃N₄ exhibits superior thermomechanical and physicochemical properties such as oxidation and thermal shock resistance, mechanical fatigue, creep and wear resistance, high fracture toughness, it is chemically inert and hydrophobic. Ge₃N₄ is known to be thermally stable and resistant to oxidation, its photocatalytic behavior has been reported. Their applications include the use for surface protection [1] (both compounds), in engine components and turbochargers, bearings, metal cutting and shaping tools and hot metal handling [2], interlayer dielectrics for metal-insulator–semiconductors devices, metal-nitride-oxide–semiconductors and as passivation films or diffusion masks [3] (Si₃N₄), in photodiodes, amplifiers [1], metal-insulator-semiconductor field effect transistors (MIS FET) [4], waveguides [5] Li-ion batteries  [6], and as photocatalysts  [7] (Ge₃N₄).

In the present study, thermal expansion of Si₃N₄ and Ge₃N₄ polymorphs is experimentally determined and discussed on the basis of literature data. Two Si₃N₄ samples and one Ge₃N₄ sample (ALDRICH) were studied.

The study was performed under low- and high-temperature conditions by X–ray diffraction, at a synchrotron–radiation source. The diffraction studies were carried out at a powder diffractometer [8] at the B2 (Hasylab/DESY) bending–magnet beamline, using the Debye–Scherrer geometry. An imaging-plate detector was applied for the data collection. The Rietveld-refinement program Fullprof 2.k (v 2.7) [9] was used for the structural analysis. The quantitative analysis yielded the following proportions of α and β polymorphs in the samples: 92:8, 9:91 (samples of Si₃N₄ ) and 27:73 (sample of Ge₃N₄). The temperature variation of lattice parameters, atomic positions and thermal expansion of α and β nitride show smooth trends. It is concluded that despite the fact that each samples was built from two phases, a combination of applied experimental conditions with the careful analysis using the Rietveld method leads to acceptable values of thermal expansion in the broad temperature range studied.

References

[1] B. Molina, L.E. Sansores, "Electronic structure of Ge₃N₄ possible structures," Int. J. Quant. Chem. 80 (2), (2000) 249-257 (Spec. Issue: Third Congress of the International Society for Theoretical Chemical Physics, Ed: M. Castro, J. Ladik, C. Bunge).

[2] R. Katz, "Commercial applications of silicon nitride based ceramics," Mater. Technol. 8 (1993) 142-148.

[3] C. Juang, J.H. Chang, R.Y. Hwang, "Properties of very low temperature plasma deposited silicon nitride films," J. Vac. Sci. Technol. B 10 (1992) 1221-1223.

[4] K.P. Pande, "Electrical characteristics and memory behavior of Ge₃N₄-GaAs MIS devices," Solid-State Electron. 25 (1982) 145-149.

[5] W. Stutius and W. Streifer, “Silicon nitride films on silicon for optical waveguides,” Appl. Opt. 16 (1977) 3218–3222.

[6] N. Pereira, M. Balasubramanian, L. Dupont, J. McBreen, L.C. Klein, G.G. Amatuccia, "The electrochemistry of germanium nitride with lithium," J. Electrochem. Soc. 150 (8), (2003) A1118-A1128.

[7] T. Watanabe, J. Sato, T. Takata, M. Hara, M. Yoshimura, H. Kobayashi, Y. Inoue, "Development of highly efficient photocatalyst, Ge₃N₄, using high pressure treatment," Nippon Kagakkai Koen Yokoshu 84 (1) (2004) 479.

[8] M. Knapp, C. Baehtz, H. Ehrenberg and H. Fuess, "The synchrotron powder diffractometer at beamline B2 at HASYLAB/DESY: status and capabilities," J. Synchrotron Rad. 11 (2004) 328-334.

[9] J. Rodriguez-Carvajal, "Recent Developments of the Program FULLPROF" IUCr Newslett. 26 (2001) pp. 12-19.

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