The layer exchange technique enables high-quality multilayer graphene (MLG) on arbitrary substrates, which is a key to combining advanced electronic devices with carbon materials. We synthesize uniform MLG layers of various thicknesses, t, ranging from 5 nm to 200 nm using Ni-induced layer exchange at 800 °C. Raman and transmission electron microscopy studies show the crystal quality of MLG is relatively low for t ≤ 20 nm and dramatically improves for t ≥ 50 nm when we prepare a diffusion controlling Al2O3 interlayer between the C and Ni layers. Hall effect measurements reveal the carrier mobility for t = 50 nm is 550 cm2/Vs, which is the highest Hall mobility in MLG directly formed on an insulator. The electrical conductivity (2700 S/cm) also exceeds a highly oriented pyrolytic graphite synthesized at 3000 °C or higher. Synthesis technology of MLG with a wide range of thicknesses will enable exploration of extensive device applications of carbon materials.

Multilayer graphene (MLG) growth on arbitrary substrates is desired for incorporating carbon wiring and heat spreaders into electronic devices. We investigated the metal-induced layer exchange growth of a sputtered amorphous C layer using Ni as a catalyst. A MLG layer uniformly formed on a SiO2 substrate at 600 °C by layer exchange between the C and Ni layers. Raman spectroscopy and electron microscopy showed that the resulting MLG layer was highly oriented and contained relatively few defects. The present investigation will pave the way for advanced electronic devices integrated with carbon materials.

The Ni-induced layer-exchange growth of amorphous carbon is a unique method used to fabricate uniform multilayer graphene (MLG) directly on an insulator. To improve the crystal quality of MLG, we prepare AlOx or SiO2 interlayers between amorphous C and Ni layers, which control the extent of diffusion of C atoms into the Ni layer. The growth morphology and Raman spectra observed from MLG formed by layer exchange strongly depend on the material type and thickness of the interlayers; a 1-nm-thick AlOx interlayer is found to be ideal for use in experiments. Transmission electron microscopy and electron energy-loss spectra reveal that the crystal quality of the resulting MLG is much higher than that of a sample without an interlayer. The grain size reaches a few μm, leading to an electrical conductivity of 1290 S/cm. The grain size and the electrical conductivity are the highest among MLG synthesized using a solid-phase reaction including metal-induced crystallization. The direct synthesis of uniform, high-quality MLG on arbitrary substrates will pave the way for advanced electronic devices integrated with carbon materials.

Metal-induced layer-exchange growth of amorphous carbon (a-C) is a unique technique for fabricating high-quality, uniform multilayer graphene (MLG) directly on an insulating material. Here, we investigated the effect of transition-metal species on the interaction between metals and a-C in the temperature range of 600–1000 °C. As a result, metals were classified into four groups: (1) layer exchange (Co, Ni, Cr, Mn, Fe, Ru, Ir, and Pt), (2) carbonization (Ti, Mo, and W), (3) local MLG formation (Pd), and (4) no graphitization (Cu, Ag, and Au). Some layer-exchange metals allowed for low-temperature MLG synthesis at 600 °C, whereas others allowed for high-quality MLG with a Raman G/D peak ratio of up to 8.3. Based on the periodic table, we constructed metal selection guidelines for growing MLG on an insulator, opening the door for applications that combine advanced electronic devices with carbon materials.

Low-temperature synthesis of multilayer graphene (MLG) on arbitrary substrates is the key to incorporating MLG-based functional thin films, including transparent electrodes, low-resistance wiring, heat spreaders, and battery anodes in advanced electronic devices. This paper reviews the synthesis of MLG via the layer exchange (LE) phenomenon between carbon and metal from its mechanism to the possibility of device applications. The mechanism of LE is completely different from that of conventional MLG precipitation methods using metals, and the resulting MLG exhibits unique features. Modulation of metal species and growth conditions enables synthesis of high-quality MLG over a wide range of growth temperatures (350 °C–1000 °C) and MLG thicknesses (5–500 nm). Device applications are discussed based on the high electrical conductivity (2700 S cm−1) of MLG and anode operation in Li-ion batteries. Finally, we discuss the future challenges of LE for MLG and its application to flexible devices.