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A technique for the in situ growth of patterned graphene by CVD has been achieved directly on insulating substrates at 800 °C. The graphene growth is catalyzed by a Ni−Cu alloy sacrificial layer, which integrates many advantages such as being lithography-free, and almost wrinkle-free, with a high repeatability and rapid growth. The etching method of the metal sacrificial layer is the core of this technique, and the mechanism is analyzed. Graphene has been found to play an important role in accelerating etching speeds. The Ni−Cu alloy exhibits a high catalytic activity, and thus, high-quality graphene can be obtained at a lower temperature. Moreover, the Ni−Cu layer accommodates a limited amount of carbon atoms, which ensures a high monolayer ratio of the graphene. The carbon solid solubility of the alloy is calculated theoretically and used to explain the experimental findings. The method is compatible with the current semiconductor process and is conducive to the industrialization of graphene devices.

Thermodynamic descriptions in databases for applications in computational thermodynamics require representation of the Gibbs energy of stable as well as metastable phases of the pure elements as a basis to model multi-component systems. In the Calphad methodology these representations are usually based on physical models.Reasonable behavior of the thermodynamic properties of phases extrapolated far outside their stable ranges is necessary in order to avoid that they become stable just because these properties extrapolate badly. This paper proposes a method to prevent crystalline solid phases in multicomponent systems to become stable again when extrapolated to temperatures far above their melting temperature.

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Carbon solid solubility in metals is an important factor affecting uniform graphene growth by chemical vapor deposition (CVD) at high temperatures. At low temperatures, however, it was found that the carbon diffusion rate (CDR) on the metal catalyst surface has a greater impact on the number and uniformity of graphene layers compared with that of the carbon solid solubility. The CDR decreases rapidly with decreasing temperatures, resulting in inhomogeneous and multilayer graphene. In the present work, a Ni–Cu alloy sacrificial layer was used as the catalyst based on the following properties. Cu was selected to increase the CDR, while Ni was used to provide high catalytic activity. By plasma-enhanced CVD, graphene was grown on the surface of Ni–Cu alloy under low pressure using methane as the carbon source. The optimal composition of the Ni–Cu alloy, 1:2, was selected through experiments. In addition, the plasma power was optimized to improve the graphene quality. On the basis of the parameter optimization, together with our previously-reported, in-situ, sacrificial metal-layer etching technique, relatively homogeneous wafer-size patterned graphene was obtained directly on a 2-inch SiO2/Si substrate at a low temperature (~600 °C).