imaging is presented as a powerful method to acquire quantitative as well as qualitative information on lowdimensional materials. The method is, however, not widely used due to limitations of the Raman scanning instruments. Here we present a hyperspectral Raman system based on Bragg tunable filtering that is capable of global imaging with significantly reduced acquisition time and improved sensitivity compared to scanning confocal Raman microscopes. The operation principles of the instrument are presented, and the performance is benchmarked using a calibrated carbon nanotube sample. Examples of various applications are shown to illustrate the abilities of the technique to characterize samples deposited on oxidized silicon substrates, including graphene stacks prepared by chemical-vapor deposition, exfoliated MoS 2 , and carbon nanotubes filled with dye molecules. The wealth of information available through this hyperspectral Raman imaging technique opens many new ways to probe the properties of complex low-dimensional materials.
We report anomalous antiresonances in the infrared spectra of doped and disordered single layer graphene. Measurements in both reflection microscopy and transmission configurations of samples grafted with halogenophenyl moieties are presented. Asymmetric transparency windows at energies corresponding to phonon modes near the Γ and K points are observed, in contrast to the featureless spectrum of pristine graphene. These asymmetric antiresonances are demonstrated to vary as a function of the chemical potential and defect density. We propose a model that involves coherent intraband scattering with defects and phonons, thus relaxing the optical selection rule forbidding access to q ≠ Γ phonons. This interpretation of the new phenomenon is supported by our numerical simulations that reproduce the experimental features.
The Drude-like response of graphene in the terahertz and infrared region of the spectrum has made it attractive for optoelectronic applications in this range, because the response can be controlled by gating and doping. [1] Graphene infrared response can further be tailored for photonics and plasmonics, as the patterned material harbors low energy plasmon modes. [2] However, the infrared spectrum of pristine single layer graphene (SLG) is monotonous; in contrast to Raman, there are no infrared-active phonon modes, while bilayer graphene displays a Fano resonance in the infrared at ~1600 cm-1. [3] In a first time, we show experimentally that grafting SLG with halogenophenyl moieties induces optical transparencies at two specific energies: 1250 and 1600 cm-1 [4], in close similarity to the bands that can also be observed in carbon nanotubes as Fano resonances. [5] Unlike bands caused by the absorption of light by vibrational modes, these antiresonances show a decrease of the absorbance, an optical transparency effect. Moreover, we show that the amplitude of the transparencies can be modulated by changing the charge carrier density through doping, and by the defect density through controlled grafting. In as second time, we will present a theory based on quantum mechanics to calculate the optical conductivity of grafted SLG. [4] The model puts into play phonon modes with momenta different from Γ that can be addressed through scattering on defects. Numerical simulations reproduce the experimental data with good agreement. The theory also captures the dependence of the signal on charge carrier density and defect density. Our findings bring a new understanding for the physics behind the infrared activity of nanostructures, while opening new capabilities for tailoring the optical spectrum of nanomaterials. References [1] Horng et al. (2011) Phys Rev B 83:165113 [2] Low & Avouris (2014) ACS Nano 8:1086 [3] Kuzmenko et al. (2009) Phys Rev Lett 103:116804 [4] Rousseau et al. (2014) arXiv preprint arxiv:1407.8141 [5] Lapointe et al. (2012) Phys Rev Lett 109:097402
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