Ultrafast Dynamics and Nonlinear Optical Responses from sp2- and sp3-Hybridized Domains in Graphene Oxide

  • Liu Z
  • Zhao X
  • Zhang X
 et al. 
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Abstract

The ultrafast relaxation dynamics and nonlinear optical response in single- and few-layered graphene oxide (GO) were studied by ultrafast optical differential transmission spectroscopy and Z-scan technique using various pump intensities. It was found that charge carriers with subpicosecond-to-picosecond dynamics from sp2-hybridized domains dominate the ultrafast response at low pump intensities, like graphene. Surprisingly, the influence of two-photon absorption from sp3-hybridized domains on the transient absorption signal becomes increasingly strong with pump intensities. On the basis of heterogeneous ultrafast dynamics of GO with saturable absorption in sp2 domains and two-photon absorption in sp3 domains, the nonlinear optical response can be tailored by manipulation of the degree and location of oxidation on GO sheets; this unravels the important role of sp3 domains in graphene optics and will facilitate the potential applications of GO in optoelectronics. The ultrafast relaxation dynamics and nonlinear optical response in single- and few-layered graphene oxide (GO) were studied by ultrafast optical differential transmission spectroscopy and Z-scan technique using various pump intensities. It was found that charge carriers with subpicosecond-to-picosecond dynamics from sp2-hybridized domains dominate the ultrafast response at low pump intensities, like graphene. Surprisingly, the influence of two-photon absorption from sp3-hybridized domains on the transient absorption signal becomes increasingly strong with pump intensities. On the basis of heterogeneous ultrafast dynamics of GO with saturable absorption in sp2 domains and two-photon absorption in sp3 domains, the nonlinear optical response can be tailored by manipulation of the degree and location of oxidation on GO sheets; this unravels the important role of sp3 domains in graphene optics and will facilitate the potential applications of GO in optoelectronics.

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Authors

  • Zhi-Bo Liu

  • Xin Zhao

  • Xiao-Liang Zhang

  • Xiao-Qing Yan

  • Ying-Peng Wu

  • Yong-Sheng Chen

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