Physical review. A/Physical review, A · 2021 · 28 citations · 48 references
Natural SciencesMaterials SciencePhysicsCondensed Matter PhysicsMaterials PhysicsNanomaterialsDensity Functional TheoryElectronic Band StructureGraphene NanomaterialsNonlinear Optical MaterialsNonlinear OpticsOptical Properties Of SolidsHarmonic GenerationHarmonic SpectraHigh-harmonic GenerationHigh-order Harmonic GenerationTight-binding ApproximationTight-binding TheoryTime-dependent Density Functional TheoryTransition Dipole Moments
We investigate the high-order harmonic generation in graphene irradiated by a linearly polarized intense laser, addressing the ellipticity or polarization properties of the harmonics. We exploit time-dependent density functional theory to calculate the harmonic spectra for a laser wavelength of 4770 nm and an intensity of 1.7 $\mathrm{TW}/{\mathrm{cm}}^{2}$, and our numerical results can qualitatively reproduce recent experimental data. Our simulations also reveal that the harmonic ellipticity depends on both the harmonic order and the orientation angle between the graphene symmetric axis and the laser polarization direction. It can reach 0.68 for the ninth-order harmonic at the orientation angle of ${20}^{\ensuremath{\circ}}$. To understand the mechanism of the high ellipticity, we develop a two-band model based on the tight-binding approximation. We may explain the ellipticity of high-order harmonic generation by investigating the transition dipole moments in the two-band model. Our theory further predicts a sensitive dependence of the harmonic ellipticity on the laser intensity for various laser wavelengths.
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