Modeling the effects of electron irradiation on graphene drums using the local activation model

We study the effects of electron irradiation on suspended graphene monolayers and graphene supported on SiO2 substrates in the range 5.0 × 1015–4.3 × 1017 electrons/cm2. The suspended graphene monolayers are exfoliated over SiO2 substrates containing micrometer-sized holes, with graphene completely covering the hole, and are referred to as graphene drums. The irradiation was performed using a scanning electron microscope at 20–25 keV electron energy. We observe a two-stage behavior for the ID/IG, ID′/IG, and ID/ID′ ratios as a function of the average distance between defects, LD, where ID, IG, and ID′ are the intensities of the Raman D, G, and D′ peaks, respectively. Good fits to the dependence of the ratios on LD are obtained using the local activation model equation. The fits are used to characterize the defects at high defect densities. We also carried out annealing studies of samples irradiated to the first stage and used an Arrhenius plot to measure activation energies for defect healing, Ea. We measured Ea = 0.90 eV for the graphene drums, consistent with the hydroxyl groups; for supported graphene, we measured Ea = 0.36 eV, consistent with hydrogen adsorbates. We also studied the surface of the drums using atomic force microscopy and found no observable holes after irradiation and annealing. Our results show that the local activation model is useful in characterizing the defects in graphene drums.