We report about investigations of time-dependent structural modifications in single-crystal graphene due to laser irradiation even at moderate power levels of 1 mW in a diffraction-limited spot. The modifications have been characterized by in situ scanning confocal Raman spectroscopy, atomic force height microscopy, and transport studies. The time evolution of the Raman spectrum reveals two different effects: on a short-time scale, dopants, initially present on the flake, are removed. The longer time scale behavior points to a laser induced gradual local decomposition of single-crystal graphene into a network of interconnected nanocrystallites with a characteristic length scale of approximately 10 nm due to bond breaking. The broken bonds offer additional docking sites for adsorbates as confirmed in transport and AFM height studies. These controlled structural modifications may for instance be valuable for enhancing the local reactivity, trimming graphene based gas sensors and generating spatially varying doping patterns.

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