Jacob C. König-Otto

Nonlinear Terahertz Absorption of Graphene Plasmons

Subwavelength graphene structures support localized plasmonic resonances in the terahertz and mid-infrared spectral regimes. The strong field confinement at the resonant frequency is predicted to significantly enhance the light-graphene interaction, which could enable nonlinear optics at low intensity in atomically thin, subwavelength devices. To date, the nonlinear response of graphene plasmons and their energy loss dynamics have not been experimentally studied. We measure and theoretically model the terahertz nonlinear response and energy relaxation dynamics of plasmons in graphene nanoribbons. We employ a terahertz pump-terahertz probe technique at the plasmon frequency and observe a strong saturation of plasmon absorption followed by a 10 ps relaxation time. The observed nonlinearity is enhanced by 2 orders of magnitude compared to unpatterned graphene with no plasmon resonance. We further present a thermal model for the nonlinear plasmonic absorption that supports the experimental results. The model shows that the observed strong linearity is caused by an unexpected red shift of plasmon resonance together with a broadening and weakening of the resonance caused by the transient increase in electron temperature. The model further predicts that even greater resonant enhancement of the nonlinear response can be expected in high-mobility graphene, suggesting that nonlinear graphene plasmonic devices could be promising candidates for nonlinear optical processing.Mohammad M. Jadidi, a Jacob C. König-Otto, 3, b Stephan Winnerl, c Andrei B. Sushkov, d H. Dennis Drew, e Thomas E. Murphy, f and Martin Mittendorff g Institute for Research in Electronics & Applied Physics, University of Maryland, College Park, MD 20742, USA Helmholtz-Zentrum Dresden-Rossendorf, PO Box 510119, D-01314 Dresden, Germany Technische Universität Dresden, 01069 Dresden, Germany Center for Nanophysics and Advanced Materials, University of Maryland, College Park, Maryland 20742, USA

Gouy phase shift of a tightly focused, radially polarized beam

Radially polarized beams represent an important member of the family of vector beams, in particular due to the possibility of using them to create strong and tightly focused longitudinal fields, a fundamental property that has been exploited by applications ranging from microscopy to particle acceleration. Since the properties of such a focused beam are intimately related to the Gouy phase shift, proper knowledge of its behavior is crucial. Terahertz microscopic imaging is used to extract the Gouy phase shift of the transverse and longitudinal field components of a tightly focused, radially polarized beam. Since the applied terahertz time-domain approach is capable of mapping the amplitude and phase of an electromagnetic wave in space, we are able to directly trace the evolution of the geometric phase as the wave propagates through the focus. We observe a Gouy phase shift of 2π for the transverse and of π for the longitudinal component. Our experimental procedure is universal and may be applied to determine the geometric phase of other vector beams, such as optical vortices, or even arbitrarily shaped and polarized propagating waves.

Slow Noncollinear Coulomb Scattering in the Vicinity of the Dirac Point in Graphene.

The Coulomb scattering dynamics in graphene in energetic proximity to the Dirac point is investigated by polarization resolved pump-probe spectroscopy and microscopic theory. Collinear Coulomb scattering rapidly thermalizes the carrier distribution in k directions pointing radially away from the Dirac point. Our study reveals, however, that, in almost intrinsic graphene, full thermalization in all directions relying on noncollinear scattering is much slower. For low photon energies, carrier-optical-phonon processes are strongly suppressed and Coulomb mediated noncollinear scattering is remarkably slow, namely on a ps time scale. This effect is very promising for infrared and THz devices based on hot carrier effects.

Universal ultrafast detector for short optical pulses based on graphene

Graphene has unique optical and electronic properties that make it attractive as an active material for broadband ultrafast detection. We present here a graphene-based detector that shows 40-picosecond electrical rise time over a spectral range that spans nearly three orders of magnitude, from the visible to the far-infrared. The detector employs a large area graphene active region with interdigitated electrodes that are connected to a log-periodic antenna to improve the long-wavelength collection efficiency, and a silicon carbide substrate that is transparent throughout the visible regime. The detector exhibits a noise-equivalent power of approximately 100 µW·Hz(-½) and is characterized at wavelengths from 780 nm to 500 µm.

Four-Wave Mixing in Landau-Quantized Graphene

For Landau-quantized graphene, featuring an energy spectrum consisting of nonequidistant Landau levels, theory predicts a giant resonantly enhanced optical nonlinearity. We verify the nonlinearity in a time-integrated degenerate four-wave mixing (FWM) experiment in the mid-infrared spectral range, involving the Landau levels LL-1, LL0 and LL1. A rapid dephasing of the optically induced microscopic polarization on a time scale shorter than the pulse duration (∼4 ps) is observed, while a complementary pump-probe experiment under the same experimental conditions reveals a much longer lifetime of the induced population. The FWM signal shows the expected field dependence with respect to lowest order perturbation theory for low fields. Saturation sets in for fields above ∼6 kV/cm. Furthermore, the resonant behavior and the order of magnitude of the third-order susceptibility are in agreement with our theoretical calculations.

Carrier Dynamics in Graphene: Ultrafast Many-Particle Phenomena

Graphene is an ideal material to study fundamental Coulomb- and phonon-induced carrier scattering processes. Its remarkable gapless and linear band structure opens up new carrier relaxation channels. In particular, Auger scattering bridging the valence and the conduction band changes the number of charge carriers and gives rise to a significant carrier multiplication - an ultrafast many-particle phenomenon that is promising for the design of highly efficient photodetectors. Furthermore, the vanishing density of states at the Dirac point combined with ultrafast phonon-induced intraband scattering results in an accumulation of carriers and a population inversion suggesting the design of graphene-based terahertz lasers. Here, we review our work on the ultrafast carrier dynamics in graphene and Landau-quantized graphene is presented providing a microscopic view on the appearance of carrier multiplication and population inversion.

Symmetry-Breaking Supercollisions in Landau-Quantized Graphene

Recent pump-probe experiments performed on graphene in a perpendicular magnetic field have revealed carrier relaxation times ranging from picoseconds to nanoseconds depending on the quality of the sample. To explain this surprising behavior, we propose a novel symmetry-breaking defect-assisted relaxation channel. This enables scattering of electrons with single out-of-plane phonons, which drastically accelerate the carrier scattering time in low-quality samples. The gained insights provide a strategy for tuning the carrier relaxation time in graphene and related materials by orders of magnitude.

Plasmonic efficiency enhancement at the anode of strip line photoconductive terahertz emitters.

We investigate strip line photoconductive terahertz (THz) emitters in a regime where both the direct emission of accelerated carriers in the semiconductor and the antenna-mediated emission from the strip line play a significant role. In particular, asymmetric strip line structures are studied. The widths of the two electrodes have been varied from 2 µm to 50 µm. The THz emission efficiency is observed to increase linearly with the width of the anode, which acts here as a plasmonic antenna giving rise to enhanced THz emission. In contrast, the cathode width does not play any significant role on THz emission efficiency.

Infrared/terahertz spectra of the photogalvanic effect in (Bi,Sb)Te based three-dimensional topological insulators

We report on the systematic study of infrared/terahertz spectra of photocurrents in (Bi,Sb)Te based three dimensional topological insulators. We demonstrate that in a wide range of frequencies, ranging from fractions up to tens of terahertz, the photocurrent is caused by the linear photogalvanic effect (LPGE) excited in the surface states. The photocurrent spectra reveal that at low frequencies the LPGE emerges due to free carrier Drude-like absorption. The spectra allow to determine the room temperature carrier mobilities in the surface states despite the presents of thermally activate residual impurities in the material bulk. In a number of samples we observed an enhancement of the linear photogalvanic effect at frequencies between 30÷60 THz, which is attributed to the excitation of electrons from helical surface to bulk conduction band states. Under this condition and applying oblique incidence we also observed the circular photogalvanic effect driven by the radiation helicity.

Nonlinear plasmonic THz absorption in graphene ribbons

We investigate the nonlinear plasmonic absorption in graphene ribbons by THz pump-probe spectroscopy. The optical nonlinearity is increased by more than one order of magnitude, which is in excellent agreement with theoretical calculations.