Joel D. Cox

Electrically tunable nonlinear plasmonics in graphene nanoislands

Nonlinear optical processes rely on the intrinsically weak interactions between photons enabled by their coupling with matter. Unfortunately, many applications in nonlinear optics are severely hindered by the small response of conventional materials. Metallic nanostructures partially alleviate this situation, as the large light enhancement associated with their localized plasmons amplifies their nonlinear response to record high levels. Graphene hosts long-lived, electrically tunable plasmons that also interact strongly with light. Here we show that the nonlinear polarizabilities of graphene nanoislands can be electrically tuned to surpass by several orders of magnitude those of metal nanoparticles of similar size. This extraordinary behaviour extends over the visible and near-infrared spectrum for islands consisting of hundreds of carbon atoms doped with moderate carrier densities. Our quantum-mechanical simulations of the plasmon-enhanced optical response of nanographene reveal this material as an ideal platform for the development of electrically tunable nonlinear optical nanodevices.

Dipole-dipole interaction between a quantum dot and a graphene nanodisk

We study theoretically the dipole-dipole interaction and energy transfer in a hybrid system consisting of a quantum dot and graphene nanodisk embedded in a nonlinear photonic crystal. In our model, a probe laser field is applied to measure the energy transfer between the quantum dot and graphene nanodisk, while a control field manipulates the energy transfer process. These fields create excitons in the quantum dot and surface plasmon polaritons in the graphene nanodisk which interact via the dipole-dipole interaction. Here, the nonlinear photonic crystal acts as a tunable photonic reservoir for the quantum dot, and is used to control the energy transfer. We have found that the spectrum of power absorption in the quantum dot has two peaks due to the creation of two dressed excitons in the presence of the dipole-dipole interaction. The energy transfer rate spectrum of the graphene nanodisk also has two peaks due to the absorption of these two dressed excitons. Additionally, energy transfer between the quantum dot and the graphene nanodisk can be switched on and off by applying a pump laser to the photonic crystal or by adjusting the strength of the dipole-dipole interaction. We show that the intensity and frequencies of the peaks in the energy transfer rate spectra can be modified by changing the number of graphene monolayers in the nanodisk or the separation between the quantum dot and graphene. Our results agree with existing experiments on a qualitative basis. The principle of our system can be employed to fabricate nanobiosensors, optical nanoswitches, and energy transfer devices.

Plasmon-assisted high-harmonic generation in graphene

High-harmonic generation in condensed-matter systems is both a source of fundamental insight into quantum electron motion and a promising candidate to realize compact ultraviolet and ultrafast light sources. While graphene is anticipated to efficiently generate high-order harmonics due to its anharmonic charge-carrier dispersion, experiments performed on extended samples using THz illumination have revealed only a weak effect. The situation is further complicated by the enormous electromagnetic field intensities required by this highly nonperturbative nonlinear optical phenomenon. Here we argue that the large light intensity required for high-harmonic generation to occur can be reached by exploiting localized plasmons in doped graphene nanostructures. We demonstrate through rigorous time-domain simulations that the synergistic combination of strong plasmonic near-field enhancement and a pronounced intrinsic nonlinearity result in efficient broadband high-harmonic generation within a single material. Our results support the strong potential of nanostructured graphene as a robust, electrically tunable platform for high-harmonic generation.

Quantum Effects in the Nonlinear Response of Graphene Plasmons

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.

Plasmon-Enhanced Nonlinear Wave Mixing in Nanostructured Graphene

Localized plasmons in metallic nanostructures have been widely used to enhance nonlinear optical effects due to their ability to concentrate and enhance light down to extreme-subwavelength scales. As alternatives to noble metal nanoparticles, graphene nanostructures can host long-lived plasmons that efficiently couple to light and are actively tunable via electrical doping. Here we show that doped graphene nanoislands present unique opportunities for enhancing nonlinear optical wave-mixing processes between two externally applied optical fields at the nanoscale. These small islands can support pronounced plasmons at multiple frequencies, resulting in extraordinarily high wave-mixing susceptibilities when one or more of the input or output frequencies coincide with a plasmon resonance. By varying the doping charge density in a nanoisland with a fixed geometry, enhanced wave mixing can be realized over a wide spectral range in the visible and near-infrared. We concentrate, in particular, on second- and thir...

Theory of graphene saturable absorption

Saturable absorption is a non-perturbative nonlinear optical phenomenon that plays a pivotal role in the generation of ultrafast light pulses. Here we show that this effect emerges in graphene at unprecedentedly low light intensities, thus opening avenues to new nonlinear physics and applications in optical technology. Specifically, we theoretically investigate saturable absorption in extended graphene by developing a non-perturbative single-particle approach, describing conduction-electron dynamics in the atomically-thin material using the two-dimensional Dirac equation for massless Dirac fermions, which is recast in the form of generalized Bloch equations. By solving the electron dynamics non-perturbatively, we account for both interband and intraband contributions to the intensity-dependent saturated conductivity and conclude that the former dominates regardless of the intrinsic doping state of the material. The results are in excellent agreement with atomistic quantum-mechanical simulations including higher-band effects. Additionally, we find that the modulation depth of saturable absorption in graphene can be electrically manipulated through an externally applied gate voltage. Our results are relevant for the development of graphene-based optoelectronic devices, as well as for applications in mode-locking and random lasers.

Plasmon-enhanced terahertz emission in self-assembled quantum dots by femtosecond pulses

A scheme for terahertz (THz) generation from intraband transition in a self-assembled quantum dot (QD) molecule coupled to a metallic nanoparticle (MNP) is analyzed. The QD structure is described as a three-level atom-like system using the density matrix formalism. The MNP with spherical geometry is considered in the quasistatic approximation. A femtosecond laser pulse creates a coherent superposition of two subbands in the quantum dots and produces localized surface plasmons in the nanoparticle which act back upon the QD molecule via dipole-dipole interaction. As a result, coherent THz radiation with a frequency corresponding to the interlevel spacing can be obtained, which is strongly modified by the presence of the MNP. The peak value of the terahertz signal is analyzed as a function of nanoparticles size, the MNP to QD distance, and the area of the applied laser field. In addition, we theoretically demonstrate that the terahertz pulse generation can be effectively controlled by making use of a train of femtosecond laser pulses. We show that by a proper choice of the parameters characterizing the pulse train a huge enhancement of the terahertz signal is obtained.

Plasmonic control of nonlinear two-photon absorption in graphene nanocomposites

Nonlinear two-photon absorption in a quantum dot-graphene nanoflake nanocomposite system has been investigated. An external laser field is applied to the nanocomposite to simultaneously observe two-photon processes in the quantum dot and excite localized surface plasmons in the graphene nanodisk. This resonance condition can be achieved by tuning the plasmon resonance frequency in the graphene nanoflake via electrostatic gating. It is found that the strong local field of the graphene plasmons can enhance and control nonlinear optical processes in the quantum dot. Specifically, we show that the two-photon absorption coefficient in the quantum dot can be switched between single- and double-peaked spectra by modifying the graphene-quantum dot separation. Two-photon processes in the quantum dot can also be switched on or off by slightly changing the gate voltage applied to the graphene. Our findings indicate that this system can be used for nonlinear optical applications such as all-optical switching, biosensing and signal processing.

Resonant Tunneling in Photonic Double Quantum Well Heterostructures

Here, we study the resonant photonic states of photonic double quantum well (PDQW) heterostructures composed of two different photonic crystals. The heterostructure is denoted as B/A/B/A/B, where photonic crystals A and B act as photonic wells and barriers, respectively. The resulting band structure causes photons to become confined within the wells, where they occupy discrete quantized states. We have obtained an expression for the transmission coefficient of the PDQW heterostructure using the transfer matrix method and have found that resonant states exist within the photonic wells. These resonant states occur in split pairs, due to a coupling between degenerate states shared by each of the photonic wells. It is observed that when the resonance energy lies at a bound photonic state and the two photonic quantum wells are far away from each other, resonant states appear in the transmission spectrum of the PDQW as single peaks. However, when the wells are brought closer together, coupling between bound photonic states causes an energy-splitting effect, and the transmitted states each have two peaks. Essentially, this means that the system can be switched between single and double transparent states. We have also observed that the total number of resonant states can be controlled by varying the width of the photonic wells, and the quality factor of transmitted peaks can be drastically improved by increasing the thickness of the outer photonic barriers. It is anticipated that the resonant states described here can be used to develop new types of photonic-switching devices, optical filters, and other optoelectronic devices.

Energy splitting of resonant photonic states in nonlinear nanophotonic double waveguides

We have studied the energy splitting of bound photonic states in Kerr-nonlinear double photonic waveguides. The structure is formed by embedding two Kerr-nonlinear photonic crystals in a linear photonic crystal. When an intense external laser field is applied to the system, two coupled waveguides are induced. These waveguides may also be induced by applying a stress field to the system. Due to the coupling between waveguides, bound states split into symmetric and antisymmetric pairs. Using the transfer matrix method we obtained expressions for these split bound states and their energy separation. We have shown that the energy splitting depends on the separation of the waveguides and the intensity of the applied laser. The energy splitting predicted by our expressions agrees well with the splitting of resonant states in simulated transmission spectra. Our findings agree qualitatively with existing experimental observations of coupled photonic wells fabricated from photonic crystals. We found that the bound...