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Using micro-Raman spectroscopy and scanning tunneling microscopy, we studythe relationship between structural distortion and electrical hole doping ofgraphene on a silicon dioxide substrate. The observed upshift of the Raman Gband represents charge doping and not compressive strain. Two independentfactors control the doping: (1) the degree of graphene coupling to thesubstrate, and (2) exposure to oxygen and moisture. Thermal annealing induces apronounced structural distortion due to close coupling to SiO2 and activatesthe ability of diatomic oxygen to accept charge from graphene. Gas flowexperiments show that dry oxygen reversibly dopes graphene; doping becomesstronger and more irreversible in the presence of moisture and over longperiods of time. We propose that oxygen molecular anions are stabilized bywater solvation and electrostatic binding to the silicon dioxide surface.

Atmospheric Oxygen Binding and Hole Doping in Deformed Graphene on a SiO2 Substrate