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The role of sp²/sp³ hybrid carbon regulation in the nonlinear optical properties of graphene oxide materials

Wang, Shuai, Dong, Yongli, He, Chunying, Gao, Yachen, Jia, Nan, Chen, Zhimin, Song, Weina
RSC advances 2017 v.7 no.84 pp. 53643-53652
Fourier transform infrared spectroscopy, Raman spectroscopy, X-ray photoelectron spectroscopy, absorbance, absorption, energy, ethanol, graphene oxide, nuclear magnetic resonance spectroscopy, oxidation, photons, stable isotopes
Rational regulation of localized sp²/sp³ hybrid carbon structure in graphene oxide systems plays a very important role in developing advanced carbon-based hybrid materials. Here, we report a simple ethanol solvothermal method toward precise control of the growth of the sp² hybrid carbon configurations/clusters in the sp³ carbon matrix so as to regulate the structure of electronic energy bands in the graphene oxide system. The results of morphology observation, XPS, solid-state ¹³C MAS NMR, FT-IR and Raman spectroscopy proved that controllable generation of the sp² hybrid carbon configurations/clusters can be achieved based on an executive oxidation/reduction strategy. Upon excitation by a 532 nm laser with 4 ns pulses, the obtained reduced graphene oxide (160-rGO-6) with a large number of sp² hybrid carbon configurations displays greater nonlinear reverse saturable absorption response and a higher nonlinear absorption coefficient β of 560 cm GW⁻¹ than graphene oxide with different oxidation degree (GO-X, X = 6, 8, 10 and 12), and reduced graphene oxide with relatively few sp² hybrid carbon configuration ratios (Y-rGO-6, Y = 80, 100, 120, 140 and 180). The significantly enhanced nonlinear reverse saturable absorption of 160-rGO-6 is attributed to the two photon absorption and excited state absorption originating from the sp² hybrid carbon configuration system.