Structural and mechanical properties of amorphous silicon carbonitride films prepared by vapor-transport chemical vapor deposition

The deposition of amorphous silicon carbonitride (a-SiCN:H) films has been successfully achieved through an in-house developed vapor-transport chemical vapor deposition (VT-CVD) technique in a nitrogenated atmosphere. Polydimethylsilane (PDMS) was used as a single-source precursor for both silicon and carbon, while NH₃ was mixed with argon to ensure the in-situ nitrogenation of the films. The chemical bonding and the atomic composition of the a-SiCN:H films were systematically investigated, as a function of their N content, by means of Fourier transform infrared spectroscopy (FTIR) and X-ray photoelectron spectroscopy (XPS). AFM was used to obtain 2-D and 3-D views of the films. The mechanical properties [(hardness (H) and Young's modulus (E)] of the freshly prepared films were investigated by the nanoindentation technique. It is shown that by controlling the NH₃/Ar gas flow ratio in the reactor, a-SiCN:H films with various N contents [(0-27) at.% range] are achieved. On the microstructural level, the increase incorporation of N in the a-SiCN:H films is found not only to lead to C atom substitution by N atoms in the local Si-C-N environment but also to an enhanced incorporation of hydrogen bonded to both Si and N. Furthermore, the increase incorporation of N in the a-SiCN:H films resulted in an increase of the average R_rms surface roughness from 4 to 12 nm. Moreover, the films became porous with pore size and density increase as a result of increasing N at.%. Ultimately, both H and E of the a-SiCN:H films were found to be sensitive to their N content, as they decrease (from ~ 17 GPa and 160 GPa to ~ 13 GPa and 136 GPa, respectively) when the N content is increased from 0 to 27 at.%. The formation of Si-N, Si-H, and N-H bonds at the detriment of the more stiff Si-C bonds is thought to account for the observed lowering of the mechanical properties of the a-SiCN:H films as their N content increased.