No Arabic abstract
The ability to tune the optical response of a material via electrostatic gating is crucial for optoelectronic applications, such as electro-optic modulators, saturable absorbers, optical limiters, photodetectors and transparent electrodes. The band structure of single layer graphene (SLG), with zero-gap, linearly dispersive conduction and valence bands, enables an easy control of the Fermi energy E$_F$ and of the threshold for interband optical absorption. Here, we report the tunability of the SLG non-equilibrium optical response in the near-infrared (1000-1700nm/0.729-1.240eV), exploring a range of E$_F$ from -650 to 250 meV by ionic liquid gating. As E$_F$ increases from the Dirac point to the threshold for Pauli blocking of interband absorption, we observe a slow-down of the photobleaching relaxation dynamics, which we attribute to the quenching of optical phonon emission from photoexcited charge carriers. For E$_F$ exceeding the Pauli blocking threshold, photobleaching eventually turns into photoinduced absorption, due to hot electrons excitation increasing SLG absorption. The ability to control both recovery time and sign of nonequilibrium optical response by electrostatic gating makes SLG ideal for tunable saturable absorbers with controlled dynamics.
Graphene nanoribbons are widely regarded as promising building blocks for next-generation carbon-based devices. A critical issue to their prospective applications is whether and to what degree their electronic structure can be externally controlled. Here, we combine simple model Hamiltonians with extensive first-principles calculations to investigate the response of armchair graphene nanoribbons to transverse electric fields. Such fields can be achieved either upon laterally gating the nanoribbon or incorporating ambipolar chemical co-dopants along the edges. We reveal that the field induces a semiconductor-to-semimetal transition, with the semimetallic phase featuring zero-energy Dirac fermions that propagate along the armchair edges. The transition occurs at critical fields that scale inversely with the width of the nanoribbons. These findings are universal to group-IV honeycomb lattices, including silicene and germanene nanoribbons, irrespective of the type of edge termination. Overall, our results create new opportunities to electrically engineer Dirac fermions in otherwise semiconducting graphene-like nanoribbons.
We present the first experimental investigation of nonlinear optical properties of graphene flakes. We find that at near infrared frequencies a graphene monolayer exhibits a remarkably high third-order optical nonlinearity which is practically independent of the wavelengths of incident light. The nonlinear optical response can be utilized for imaging purposes, with image contrasts of graphene which are orders of magnitude higher than those obtained using linear microscopy.
Optical harmonic generation occurs when high intensity light ($>10^{10}$W/m$^{2}$) interacts with a nonlinear material. Electrical control of the nonlinear optical response enables applications such as gate-tunable switches and frequency converters. Graphene displays exceptionally strong-light matter interaction and electrically and broadband tunable third order nonlinear susceptibility. Here we show that the third harmonic generation efficiency in graphene can be tuned by over two orders of magnitude by controlling the Fermi energy and the incident photon energy. This is due to logarithmic resonances in the imaginary part of the nonlinear conductivity arising from multi-photon transitions. Thanks to the linear dispersion of the massless Dirac fermions, ultrabroadband electrical tunability can be achieved, paving the way to electrically-tuneable broadband frequency converters for applications in optical communications and signal processing.
We use a tight-binding model and the random-phase approximation to study the Coulomb excitations in simple-hexagonal-stacking multilayer graphene and discuss the field effects. The calculation results include the energy bands, the response functions, and the plasmon dispersions. A perpendicular electric field is predicted to induce significant charge transfer and thus capable of manipulating the energy, intensity, and the number of plasmon modes. This could be further validated by inelastic light scattering or electron-energy-loss spectroscopy.
The possibility of triggering correlated phenomena by placing a singularity of the density of states near the Fermi energy remains an intriguing avenue towards engineering the properties of quantum materials. Twisted bilayer graphene is a key material in this regard because the superlattice produced by the rotated graphene layers introduces a van Hove singularity and flat bands near the Fermi energy that cause the emergence of numerous correlated phases, including superconductivity. While the twist angle-dependence of these properties has been explored, direct demonstration of electrostatic control of the superlattice bands over a wide energy range has, so far, been critically missing. This work examines a functional twisted bilayer graphene device using in-operando angle-resolved photoemission with a nano-focused light spot. A twist angle of 12.2$^{circ}$ is selected such that the superlattice Brillouin zone is sufficiently large to enable identification of van Hove singularities and flat band segments in momentum space. The doping dependence of these features is extracted over an energy range of 0.4 eV, expanding the combinations of twist angle and doping where they can be placed at the Fermi energy and thereby induce new correlated electronic phases in twisted bilayer graphene.