The Realistic Domain Structure of As-Synthesized Graphene Oxide from Ultrafast Spectroscopy

Graphene oxide (GO) is an attractive alternative for large-scale production of graphene, but its general structure is still under debate due to its complicated nonstoichiometric nature. Here we perform a set of femtosecond pump–probe experiments on as-synthesized GO to extrapolate structural information in situ. Remarkably, it is observed that, in these highly oxidized GO samples, the ultrafast graphene-like dynamics intrinsic to pristine graphene is completely dominant over a wide energy region and can be modified by the localized impurity states and the electron–phonon coupling under certain conditions. These observations, combined with the X-ray photoelectron spectroscopy analysis and control experiments, lead to an important conclusion that GO consists of two types of domain, namely the carbon-rich graphene-like domain and the oxygen-rich domain. This study creates a new understanding of the realistic domain structure and properties of as-synthesized GO, offering useful guidance for future applications based on chemically modified/functionalized graphenes.