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We demonstrate an ultrafast reversible modulation of resonant terahertz (THz) response in strongly photoexcited metamaterials. The transient spectral-temporal response of the dipole transition ~1.6 THz exhibits a distinct non-monotonic variation as a function of pump fluence. The transition energy shift, strength, spectral width and density-dependent ultrafast relaxation manifest a remarkable re-emergence of the resonances after initial quenching. Our simulation, incorporating the first-order diffraction from the photoinduced transient grating, reproduces the salient features, providing a new avenue for designing nonlinear and frequency-agile THz modulators.

We report the synthesis and evidence of graphene fluoride, a two-dimensional wide bandgap semiconductor derived from graphene. Graphene fluoride exhibits hexagonal crystalline order and strongly insulating behavior with resistance exceeding 10 G$\Omega$ at room temperature. Electron transport in graphene fluoride is well described by variable-range hopping in two dimensions due to the presence of localized states in the band gap. Graphene obtained through the reduction of graphene fluoride is highly conductive, exhibiting a resistivity of less than 100 k$\Omega$ at room temperature. Our approach provides a new path to reversibly engineer the band structure and conductivity of graphene for electronic and optical applications., Comment: 7 pages, 5 figures, revtex, to appear in PRB