Since 2008, epitaxial graphene growth has been developed in terms of homogeneity and scale by using a 1 ATM argon pressure at high temperature (>1650°C). Until now, it still remains challenging to obtain films with different and controlled characteristics such as the thickness or the doping by tuning the growth parameters. Here, we optimized the epitaxial growth of monolayer graphene (1LG) on 4H-SiC (0001) under a low argon pressure of 10 mbar. This intermediate pressure allows growing a continued 1LG in a short process ~1h30.
First, we discuss the initial growth stages from buffer layer to 1LG as a function of annealing temperature (same heating rate). The combined Raman spectroscopy and atomic force microscopy analyses show that a buffer layer, fully covering the Si-face of SiC, forms as the first step of growth. Subsequently, 1LG starts to grow at step edges and continue to cover the buffer layer on terraces with a step-flow growth mechanism. Eventually, reproducible syntheses of 1LG films were achieved by this temperature-controlled growth process. Then, we investigate the structural and electronic properties of the 1LG films. The integrated intensity of G-band in Raman spectra normalized with respect to a HOPG reference, AG/AG-HOPG, of each spectrum in Raman map of our continued graphene film is very close to the experimental value reported for a 1LG, demonstrating the good homogeneity. Atomically resolved scanning tunnelling
microscopy (STM) evidences a (6x6) superstructure, indicative of 1LG covering a reconstructed interface layer[7]. Regarding the transport measurement, quantum Hall plateau values observed in our graphene layers confirmed both continuity and thickness of the
1LG film. Moreover, we estimated a hole concentration of p~10^10 - 10^11 /(cm^2) at 1.7 K in helium atmosphere. We ascribe this unusual doping type to an atmosphere contamination effect since we regain the typical n-doped graphene under vacuum by transport measurement and STM analysis.