As a kind of protective material, Diamond-Like Carbon (DLC) film can effectively improve the mechanical and tribological properties of the substrate surface. In DLC family, tetrahedral amorphous carbon (ta-C) with ultra-high hardness and excellent protective properties has been widely concerned in the field of hard protective materials. It is well known that the structure and properties of ta-C are strongly dependent on carbon plasma characteristics in the plasma environment. Therefore, it is extremely crucial to obtain the optimal process window of ta-C described by plasma micro-parameters with general significance. This paper proposed the Langmuir probe was used to diagnose the carbon plasma of the afterglow generated by arc evaporation, aiming to investigate the characteristics of carbon plasma and sheath. The effect of ion energy and ion flux adjusted by the pulse bias voltage and arc current on the sp3 hybrid bonds and hardness of DLC films was studied, aiming to find out which conditions satisfied the formation of ta-C. The results showed the microstructure and properties of DLC films were co-adjusted by ion energy and ion flux. When the carbon ions met the appropriate ion energy range (50–300 eV) and low ion flux (<8.99 × 1010 cm−2 s−1), the films tended to form ta-C structures with high sp3 bonds. However, under the condition of high ion energy and high ion flux, the structure of the films changed from sp3 bonds to sp2 bonds, resulting in the graphitization and formation of DLC films with high sp2 bonds. This work will provide new solutions to guide the design and acquisition of high-performance DLC films.
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