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Register a new userA study of the nonlinear optical response of the plain graphene and gapped graphene monolayers beyond the Dirac approximation
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Added by
Gon\\c{c}alo Ventura
Publication date
2019
fields
Physics
and research's language is
English
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In this work, we present numerical results for the second and third order conductivities of the plain graphene and gapped graphene monolayers associated with the second and third harmonic generation, the optical rectification and the optical Kerr effect. The frequencies considered here range from the microwave to the ultraviolet portion of the spectrum, the latter end of which had not yet been studied. These calculations are performed in the velocity gauge and directly address the components of the conductivity tensor. In the velocity gauge, the radiation field is represented by a power series in the vector potential, and we discuss a very efficient way of calculating its coefficients in the context of tight-binding models.
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Materials with massless Dirac fermions can possess exceptionally strong and widely tunable optical nonlinearities. Experiments on graphene monolayer have indeed found very large third-order nonlinear responses, but the reported variation of the nonlinear optical coefficient by orders of magnitude is not yet understood. A large part of the difficulty is the lack of information on how doping or chemical potential affects the different nonlinear optical processes. Here we report the first experimental study, in corroboration with theory, on third harmonic generation (THG) and four-wave mixing (FWM) in graphene that has its chemical potential tuned by ion-gel gating. THG was seen to have enhanced by ~30 times when pristine graphene was heavily doped, while difference-frequency FWM appeared just the opposite. The latter was found to have a strong divergence toward degenerate FWM in undoped graphene, leading to a giant third-order nonlinearity. These truly amazing characteristics of graphene come from the possibility to gate-control the chemical potential, which selectively switches on and off one- and multi-photon resonant transitions that coherently contribute to the optical nonlinearity, and therefore can be utilized to develop graphene-based nonlinear optoelectronic devices.
The ability of graphene to support long-lived, electrically tunable plasmons that interact strongly with light, combined with its highly nonlinear optical response, has generated great expectations for application of the atomically-thin material to nanophotonic devices. These expectations are mainly reinforced by classical analyses performed using the response derived from extended graphene, neglecting finite-size and nonlocal effects that become important when the carbon layer is structured on the nanometer scale in actual device designs. Here we show that finite-size effects produce large contributions that increase the nonlinear response of nanostructured graphene to significantly higher levels than those predicted by classical theories. We base our analysis on a quantum-mechanical description of graphene using tight-binding electronic states combined with the random-phase approximation. While classical and quantum descriptions agree well for the linear response when either the plasmon energy is below the Fermi energy or the size of the structure exceeds a few tens of nanometers, this is not always the case for the nonlinear response, and in particular, third-order Kerr-type nonlinearities are generally underestimated by the classical theory. Our results reveal the complex quantum nature of the optical response in nanostructured graphene, while further supporting the exceptional potential of this material for nonlinear nanophotonic devices.
We study theoretically the interaction of ultrashort optical pulses with gapped graphene. Such strong pulse results in finite conduction band population and corresponding electric current both during and after the pulse. Since gapped graphene has broken inversion symmetry, it has an axial symmetry about the $y$-axis but not about the $x$-axis. We show that, in this case, if the linear pulse is polarized along the $x$-axis, the rectified electric current is generated in the $y$ direction. At the same time, the conduction band population distribution in the reciprocal space is symmetric about the $x$-axis. Thus, the rectified current in gapped graphene has inter-band origin, while the intra-band contribution to the rectified current is zero.
We present realistic simulations of quantum confinement effects in ballistic graphene quantum dots with linear dimensions of 10 to 40 nm. We determine wavefunctions and energy level statistics in the presence of disorder resulting from edge roughness, charge impurities, or short-ranged scatterers. Marked deviations from a simple Dirac billiard for massless fermions are found. We find a remarkably stable dependence of the nearest-neighbor level spacing on edge roughness suggesting that the roughness of fabricated devices can be potentially characterized by the distribution of measured Coulomb blockade peaks.
Second-order nonlinear optical response allows to detect different properties of the system associated with the inversion symmetry breaking. Here, we use a second harmonic generation effect to investigate the alignment of a graphene/hexagonal Boron Nitride heterostructure. To achieve that, we activate a commensurate-incommensurate phase transition by a thermal annealing of the sample. We find that this structural change in the system can be directly observed through a strong modification of a nonlinear optical signal. This result reveals the potential of a second harmonic generation technique for probing structural properties of layered systems.
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