Influence of Chemisorbed Oxygen on the Growth of Graphene on Cu(100) by Chemical Vapor Deposition

Abstract

Understanding the influence that copper substrate surface symmetry and oxygen impurities have on the growth of graphene by chemical vapor deposition is important for developing techniques for producing high quality graphene. Therefore, we have studied the growth of graphene by catalytic decomposition of ethylene in an ultra-high vacuum chamber on both a clean Cu(100) surface and a Cu(100) surface pre-dosed with a layer of chemisorbed oxygen. The crystal structure of the graphene films was characterized with \emph{in-situ} low energy electron diffraction. By heating the clean Cu(100) substrate from room temperature to the growth temperature in ethylene, epitaxial graphene films were formed. The crystal quality was found to depend strongly on the growth temperature. At 900 $^\circ$C, well-ordered two-domain graphene films were formed. Pre-dosing the Cu(100) surface with a chemisorbed layer of oxygen before graphene growth was found to adversely affect the crystal quality of the graphene overlayer by inducing a much higher degree of rotational disorder of the graphene grains with respect to the Cu(100) substrate. The growth morphology of the graphene islands during the initial stages of nucleation was monitored with \emph{ex-situ} scanning electron microscopy. The nucleation rate of the graphene islands was observed to drop by an order of magnitude by pre-dosing the Cu(100) surface with a chemisorbed oxygen layer before growth. This reduction in nucleation rate results in the formation of much larger graphene islands. Therefore, the presence of oxygen during graphene growth affects both the relative orientation and average size of grains within the films grown on Cu(100) substrates.