A range of amorphous hydrogenated silicon-carbide films have been produced using the plasma-enhanced chemical-vapour deposition technique with silane and methane diluted in hydrogen as the parent molecules. The air-exposed and sputtercleaned surfaces of these films have been investigated by means of X-ray photoelectron spectroscopy. Auger electron spectroscopy, secondary-ion mass spectrometry, Raman spectroscopy and reflection-electron diffraction. The structural and chemical nature of the films has been determined as a function of the methane: silane ratio by a combination of the above techniques. X-ray photoelectron spectroscopy and Auger electron spectroscopy have been used to determine the carbon content of the films also as a function of the methane : silane ratio. § 1. INTRODUCTION Hydrogenated amorphous binary alloys, such as amorphous hydrogenated silicon carbide (a-Sic : H), have proved to be attractive materials with applications to solar cells, photoreceptors and graphic devices (Tarui et al. 1987, Tawada, Kondo, Okamoto andHamakawa 1982). These applications result from the fact that their optical gap can be continuously controlled by varying the alloy compositional ratio (Anderson and Spear 1977).It is has been shown that the optical and electronic properties of these films are a sensitive function of the specific bonding configurations present (Fukada et al. 1983) as well as the alloy composition. In the light of this, it is important to develop a more detailed fundamental understanding of the structure and bonding configurations of these films over the composition range.A previous investigation of a-Si, -xCx : H prepared by plasma-enhanced chemical vapour deposition (PECVD) of methane (CH,) and silane (SiH,) has been undertaken by Lee (1980). The techniques of X-ray photoelectron spectroscopy (XPS), Auger electron spectroscopy (AES) and reported infrared spectroscopy were used to characterize the films. The main conclusions of the study were that the structure of PECVD a-Sic : H films containing less than 70% carbon is best described in terms of a t slightly cross-linked, carbon-and hydrogen-substituted polysilicon. Once the carbon content exceeds this value one obtains an almost fully cross-linked, silicon-and hydrogen-substituted polycarbon.As compared to a-Si : H, the a-Sic : H films produced using the conventional PECVD technique possess inferior photoelectric properties. Recently it has been demonstrated (Matsuda et al. 1986) that H, dilution of the starting SiH, : CH, mixture leads to highly photosensitive films with photoconductivities up to three orders of magnitude greater than their non-diluted counterparts (Matsuda and Tanaka 1987).These results stimulated the following detailed investigation aimed at relating structural, chemical and compositional data with the optical and electronic properties of the same range of specimens. The a-Si,-,C,:H films were deposited in a conventional glow discharge reactor over a range from x=O*1 to 0-7 with different H, dilutions. The structural, chemical ...