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Register a new userLarge nonlinear Kerr effect in graphene
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Under strong laser illumination, few-layer graphene exhibits both a transmittance increase due to saturable absorption and a nonlinear phase shift. Here, we unambiguously distinguish these two nonlinear optical effects and identify both real and imaginary parts of the complex nonlinear refractive index of graphene. We show that graphene possesses a giant nonlinear refractive index n2=10-7cm2W-1, almost nine orders of magnitude larger than bulk dielectrics. We find that the nonlinear refractive index decreases with increasing excitation flux but slower than the absorption. This suggests that graphene may be a very promising nonlinear medium, paving the way for graphene-based nonlinear photonics.
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We introduce the concept of nonlinear graphene metasurfaces employing the controllable interaction between a graphene layer and a planar metamaterial. Such hybrid metasurfaces support two types of subradiant resonant modes, asymmetric modes of structured metamaterial elements (metamolecules) and graphene plasmons exhibiting strong mutual coupling and avoided dispersion crossing. High tunability of graphene plasmons facilitates strong interaction between the subradiant modes, modifying the spectral position and lifetime of the associated Fano resonances. We demonstrate that strong resonant interaction, combined with the subwavelength localization of plasmons, leads to the enhanced nonlinear response and high efficiency of the second-harmonic generation.
By means of the ultrafast optical Kerr effect method coupled to optical heterodyne detection (OHD-OKE), we characterize the third order nonlinear response of graphene at telecom wavelength, and compare it to experimental values obtained by the Z-scan method on the same samples. From these measurements, we estimate a negative nonlinear refractive index for monolayer graphene, $n_2 = - 1.1times 10^{-13} m^2/W$. This is in contradiction to previously reported values, which leads us to compare our experimental measurements obtained by the OHD-OKE and the Z-scan method with theoretical and experimental values found in the literature, and to discuss the discrepancies, taking into account parameters such as doping.
In magnetoplasmonics, it is possible to tailor the magneto-optical properties of nanostructures by exciting surface plasmon polaritons (SPPs). Thus far, magnetoplasmonic effects have been considered static. Here, we describe ultrafast manifestations of magnetoplasmonics by observing the non-trivial evolution of the transverse magneto-optic Kerr effect within 45-fs pulses reflected from an iron-based magnetoplasmonic crystal. The effect occurs for resonant SPP excitations, displays opposite time derivative signs for different slopes of the resonance, and is explained with the magnetization-dependent dispersion relation of SPPs.
The formation of a superstructure - with a related Moire pattern - plays a crucial role in the extraordinary optical and electronic properties of twisted bilayer graphene, including the recently observed unconventional superconductivity. Here we put forward a novel, interdisciplinary approach to determine the Moire angle in twisted bilayer graphene based on the photonic spin Hall effect. We show that the photonic spin Hall effect exhibits clear fingerprints of the underlying Moire pattern, and the associated light beam shifts are well beyond current experimental sensitivities in the near-infrared and visible ranges. By discovering the dependence of the frequency position of the maximal photonic spin Hall effect shift on the Moire angle, we argue that the latter could be unequivocally accessed via all-optical far-field measurements. We also disclose that, when combined with the Goos-Hanchen effect, the spin Hall effect of light enables the complete determination of the electronic conductivity of the bilayer. Altogether our findings demonstrate that sub-wavelength spin-orbit interactions of light provide a unprecedented toolset for investigating optoelectronic properties of multilayer two-dimensional van der Waals materials.
Nonlinear optics is an increasingly important field for scientific and technological applications, owing to its relevance and potential for optical and optoelectronic technologies. Currently, there is an active search for suitable nonlinear material systems with efficient conversion and small material footprint. Ideally, the material system should allow for chip-integration and room-temperature operation. Two-dimensional materials are highly interesting in this regard. Particularly promising is graphene, which has demonstrated an exceptionally large nonlinearity in the terahertz regime. Yet, the light-matter interaction length in two-dimensional materials is inherently minimal, thus limiting the overall nonlinear-optical conversion efficiency. Here we overcome this challenge using a metamaterial platform that combines graphene with a photonic grating structure providing field enhancement. We measure terahertz third-harmonic generation in this metamaterial and obtain an effective third-order nonlinear susceptibility with a magnitude as large as 3$cdot$10$^{-8}$m$^2$/V$^2$, or 21 esu, for a fundamental frequency of 0.7 THz. This nonlinearity is 50 times larger than what we obtain for graphene without grating. Such an enhancement corresponds to third-harmonic signal with an intensity that is three orders of magnitude larger due to the grating. Moreover, we demonstrate a field conversion efficiency for the third harmonic of up to $sim$1% using a moderate field strength of $sim$30 kV/cm. Finally we show that harmonics beyond the third are enhanced even more strongly, allowing us to observe signatures of up to the 9$^{rm th}$ harmonic. Grating-graphene metamaterials thus constitute an outstanding platform for commercially viable, CMOS compatible, room temperature, chip-integrated, THz nonlinear conversion applications.
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