The low-energy (intraband) range of the third harmonic generation of graphene in the terahertz regime is governed by the damping terms induced by the interactions. A controlled many-body description of the scattering processes is thus a compelling and desirable requirement. In this paper, using a Kadanoff-Baym approach, we systematically investigate the impact of many-body interaction on the third-harmonic generation (THG) of graphene, taking elastic impurity scattering as a benchmark example. We predict the onset in the mixed inter-intraband regime of novel incoherent features driven by the interaction at four- and five-photon transition frequencies in the third-harmonic optical conductivity with a spectral weight proportional to the scattering rate.We show also that, in spite of the complex many-body physics, the purely intraband term governing the limit $ω\to 0$ resembles the constraints of the phenomenological model. We ascribe this agreement to the fulfilling of the conservation laws enforced by the conserving approach. The overlap with novel incoherent features and the impact of many-body driven multi-photon vertex couplings limit however severely the validity of phenomenological description.
Higher harmonic generation in plane graphene quantum dots initiated by intense coherent radiation is investigated, using dynamical Hartree-Fock mean-field theory. A microscopic theory describing the extreme nonlinear optical response of plane graphene quantum dots is developed. The closed set of differential equations for the single-particle density matrix at the graphene quantum dots-strong laser field multiphoton interaction is solved numerically. The obtained solutions indicate the significance of the type of edge and lateral size, and bandgap and laser field strength in the high harmonic g…
Generation of high harmonics in a monolayer graphene initiated by strong coherent radiation field, taking into account electron-electron Coulomb interaction is investigated. A microscopic theory describing the nonlinear optical response of graphene is developed. The Coulomb interaction of electrons is treated in the scope of dynamic Hartree-Fock approximation. The closed set of integrodifferential equations for the single-particle density matrix of a graphene quantum structure is solved numerically. The obtained solutions show the significance of many-body Coulomb interaction on the high harmo…
Using the microscopic nonlinear quantum theory of interaction of strong coherent electromagnetic radiation with a gapped bilayer graphene is developed for high harmonic generation at low-energy photon excitation-induced Lifshitz transitions. The Liouville-von Neumann equation for the density matrix is solved numerically at the nonadiabatic multiphoton excitation regime. By numerical solutions, we examine the rates of the second and third harmonics generation at the particle-hole annihilation in induced Lifshitz transitions by the two linearly polarized coherent electromagnetic waves propagatin…
We propose a novel method for controlling the high-harmonic generation (HHG) with a high dynamic range in single-layer graphene. We find that, by utilizing shear strain, a significant enhancement or quenching of HHG is possible over a range of several orders of magnitude. This feature is made possible by the resonance mechanism at a van Hove singularity. Therein, the shear strain controls the configurations of the two Dirac cones, resulting in changes in the energy and dipole moment at the saddle point of the band dispersion. Our findings provide a way for modulating or switching light by usin…
Microscopic nonlinear quantum theory of interaction of coherent electromagnetic radiation with gapped bilayer graphene is developed. The Liouville-von Neumann equation for the density matrix is solved numerically at the multiphoton excitation regime. The developed theory of interaction of charged carriers with strong driving wave field is valid near the Dirac points of the Brillouin zone. We consider the harmonic generation process in the nonadiabatic regime of interaction when the Keldysh parameter is of the order of unity. On the basis of numerical solutions, we examine the rates of odd and …
We observe enhanced second-harmonic generation in monolayer graphene in the presence of an ultra-strong terahertz field pulse with a peak amplitude of 250 kV/cm. This is a strongly nonperturbative regime of light-matter interaction in which particles get accelerated to energies exceeding the initial Fermi energy of 0.2 eV over a timescale of a few femtoseconds. The second-harmonic current is generated as electrons drift through the region of momenta corresponding to interband transition resonance at an optical frequency. The resulting strongly asymmetric distortion of carrier distribution in m…
The higher order harmonic generation process in the nonperturbative regime at the interaction of coherent electromagnetic radiation with the AB-stacked bilayer graphene at high Fermi energies is considered. The applied coherent low-frequency radiation field in the high Fermi energy zone of electrons excludes the interband transitions enhancing high harmonic rates. The developed microscopic nonlinear quantum theory for charged carriers interaction with a strong pump wave is valid near the Dirac points of the Brillouin zone. The Liouville-von Neumann equation for the density matrix in the multip…
For centrosymmetric materials such as monolayer graphene, no optical second harmonic generation (SHG) is generally expected because it is forbidden under the electric-dipole approximation. Yet we observed a strong, doping induced SHG from graphene, with its highest strength comparable to the electric-dipole allowed SHG in non-centrosymmetric 2D materials. This novel SHG has the nature of an electric-quadrupole response, arising from the effective breaking of inversion symmetry by optical dressing with an in-plane photon wave vector. More remarkably, the SHG is widely tuned by carrier doping or…
High-order frequency mixing in graphene using a two-color radiation field consisting of the fundamental and the second harmonic fields of an ultrashort linearly polarized laser pulse is studied. It is shown that the harmonics originated from the interband transitions are efficiently generated in the case of the orthogonally polarized two-color field. In this case, the generated high-harmonics are stronger than those obtained in the parallel polarization case by more than two orders of magnitude. This is in sharp contrast with the atomic and semiconductor systems, where parallel polarization ca…
Crystal symmetry plays a central role in governing a wide range of fundamental physical phenomena. One example is the nonlinear optical second harmonic generation (SHG), which requires inversion symmetry breaking. Here we report a unique stacking-induced SHG in trilayer graphene, whose individual monolayer sheet is centrosymmetric. Depending on layer stacking sequence, we observe a strong optical SHG in Bernal (ABA) stacked non-centrosymmetric trilayer, while it vanishes in rhombohedral (ABC) stacked one which preserves inversion symmetry. This highly contrasting SHG due to the distinct stacki…
Resonant Structure of Second Harmonic Generation in Multilayer Graphene Polytypes
National Graphene Institute, University of Manchester（国家石墨烯研究所，曼彻斯特大学）；Department of Physics & Astronomy, University of Manchester（曼彻斯特大学物理与天文系）；Department of Physics, University of Osaka（大阪大学物理系）
Two-dimensional materials constitute an exciting platform for nonlinear optics with large nonlinearities that are tunable by gating. Hence, gate-tunable harmonic generation and intensity-dependent refraction have been observed in e.g. graphene and transition-metal dichalcogenides, whose electronic structures are accurately modelled by the (massive) Dirac equation. We exploit on the simplicity of this model and demonstrate here that arbitrary nonlinear response functions follow from a simple iterative approach. The power of this approach is illustrated by analytical expressions for harmonic gen…
We model the magnetic ratchet effect in bilayer graphene in which a dc electric current is produced by an ac electric field of frequency $ω$ in the presence of a steady in-plane magnetic field and inversion-symmetry breaking. In bilayer graphene, the ratchet effect is tunable by an external metallic gate which breaks inversion symmetry. For zero in-plane magnetic field, we show that trigonal warping and inversion-symmetry breaking are able to produce a large dc valley current, but not a non-zero total dc charge current. For the magnetic ratchet in a tilted magnetic field, the perpendicular fie…
An optical Second-Harmonic Generation (SHG) allows to probe various structural and symmetry-related properties of materials, since it is sensitive to the inversion symmetry breaking in the system. Here, we investigate the SHG response from a single layer of graphene disposed on an insulating hexagonal Boron Nitride (hBN) and Silicon Carbide (SiC) substrates. The considered systems are described by a non-interacting tight-binding model with a mass term, which describes a non-equivalence of two sublattices of graphene when the latter is placed on a substrate. The resulting SHG signal linearly de…
We investigate high-harmonic generation in graphene heterostructures consisting of metallic nanoribbons separated from a graphene sheet by either a few-nanometer layer of aluminum oxide or an atomic monolayer of hexagonal boron nitride. The nanoribbons amplify the near-field at the graphene layer relative to the externally applied pumping, thus allowing us to observe third- and fifth-harmonic generation in the carbon monolayer at modest pump powers in the mid-infrared. We study the dependence of the nonlinear signals on the ribbon width and spacer thickness, as well as pump power and polarizat…
Nonlinear nanophotonics leverages engineered nanostructures to funnel light into small volumes and intensify nonlinear optical processes with spectral and spatial control. Due to its intrinsically large and electrically tunable nonlinear optical response, graphene is an especially promising nanomaterial for nonlinear optoelectronic applications. Here we report on exceptionally strong optical nonlinearities in graphene-insulator-metal heterostructures, demonstrating an enhancement by three orders of magnitude in the third-harmonic signal compared to bare graphene. Furthermore, by increasing the…
Due to its linear dispersion, monolayer graphene is expected to generate a third harmonic response at terahertz frequencies. There have been a variety of different models of this effect and recently it has been experimentally observed. However, there is still considerable uncertainty as to the role of scattering on harmonic generation in graphene. In this work, we model third-harmonic generation in doped monolayer graphene at THz frequencies by employing a nearest-neighbour tight-binding model in the length gauge. We include optical phonon and neutral impurity scattering at the microscopic lev…
High-harmonic generation (HHG) in solids is an emerging method to probe ultrafast electron dynamics in solids at attosecond timescale. In this work, we study HHG from monolayer and bilayer graphene. Bilayer graphenes with AA and AB stacking are considered in this work. It is found that the monolayer and bilayer graphenes exhibit significantly different harmonic spectra. The difference in the spectra is attributed to the interlayer coupling between the two layers. Also, the intraband and interband contributions to the total harmonic spectrum play a significant role. Moreover, interesting polari…
Third nearest neighbor parameterized tight biding model for graphene nano-ribbons
由Reich等人提出的第三近邻紧束缚模型[Phys. Rev. B 66，035412]很好地再现了2D石墨烯片的从头算能带结构。对于带状结构，现有的紧束缚参数组可以成功地解释所有扶手椅型带状结构的半导体行为。然而，他们仍然无法准确地描述带的斜率，而这个特征与电子的群速度和有效质量直接相关。在这项工作中，两个密度泛函理论和紧束缚计算进行，并介绍了一套新的紧束缚参数的第三近邻包括重叠条款。用这个模型得到的结果提供极好的协议与密度泛函理论的预测在大多数情况下的带状结构，即使在高能量区。此外，这套可以诱导电子空穴不对称性，表现在密度泛函理论。相关的结果也证明了扶手椅带的各种宽度，以及锯齿形结构，从而开辟了多尺度模拟的路线。
We study narrow zigzag graphene nanoribbons (ZGNRs), employing density functional theory (DFT) simulations and the tight-binding (TB) method. The main result of these calculations is the braiding of the conduction and valence bands, generating Dirac cones for non-commensurate wave vectors $\vec{k}$. Employing a TB Hamiltonian, we show that the braiding is generated by the third-neighbor hopping (N3). We calculate the band structure, the density of states and the conductance, new conductance channels are opened, and the conductance at the Fermi energy assumes integer multiples of the quantum co…
Hot electrons dominate the ultrafast ($\sim$fs-ps) optical and electronic properties of metals and semiconductors and they are exploited in a variety of applications including photovoltaics and photodetection. We perform power-dependent third harmonic generation measurements on gated single-layer graphene and detect a significant deviation from the cubic power-law expected for a third harmonic generation process. We assign this to the presence of hot electrons. Our results indicate that the performance of nonlinear photonics devices based on graphene, such as optical modulators and frequency c…
The generation of high-order harmonics in quasi-one-dimensional graphene nanoribbons (GNRs) initiated by intense coherent radiation is investigated. A microscopic theory describing the extreme nonlinear optical response of GNRs is developed. The closed set of differential equations for the single-particle density matrix at the GNR-strong laser field multiphoton interaction is solved numerically. The obtained solutions indicate the significance of the bandgap width and Fermi energy level on the high-order harmonic generation process in GNRs.
Static Non-linearity in Graphene Field Effect Transistors
研究了GFET跨导器的静态线性性能指标，并建立了模型。给出了二阶和三阶谐波失真（HD 2、HD 3）、二阶和三阶互调失真（Δ IM 2、Δ IM 3）以及二阶和三阶交截点（AIIP 2、AIIP 3）的闭合表达式。通过使用GFET VerilogA分析模型和商业电路模拟器的大信号仿真验证的表达式。所提出的表达式可以在电路设计过程中使用，以预测GFET的偏置条件下，满足线性度要求。
