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The growth and characteristics of metal containing §amorphous hydrogenated carbon thin films (a-C:H/Me) §were studied in this research. The discovery and the §explanation of unprecedented self-assembled, §alternating nano-layered structures are addressed. a-§C:H/Me thin films were synthesized using one single §target, a rotating but not revolving substrate, and §constant feed gas compositions in a conventional §reactive sputter deposition chamber. In order to §explain the formation of the distinct structures, §correlations were first made among the deposition §rate, the composition, the crystallinity, the §surface chemistry, and the microstructure of a-§C:H/Me thin films. As a result, a processing window §was obtained for the formation of the self-§assembled, alternating nano-layered structures. It §was found that such structures can be obtained under §controlled growth parameters for selected metals. A §growth mechanism based on the considerations of §clustering of carbon and metal, segregation of §carbon, catalytic effects of metal, formation of §carbide, energy of adatoms, and surface diffusion of §metal and carbon, has been developed.