Terahertz photoresponse of black phosphorus.

Two-dimensional black phosphorus is a new material that has gained widespread interest as an active material for optoelectronic applications. It features high carrier mobility that allows for efficient free-carrier absorption of terahertz radiation, even though the photon energy is far below the bandgap energy. Here we present an efficient and ultrafast terahertz detector, based on exfoliated multilayer flakes of black phosphorus. The device responsivity is about 1 mV/W for a 2.5 THz beam with a diameter of 200 µm, and is primarily limited by the small active area of the device in comparison to the incident beam area. The intrinsic responsivity is determined by Joule heating experiments to be about 44 V/W, which is in agreement with predictions from the Drude conductivity model. Time resolved measurements at a frequency of 0.5 THz reveal an ultrafast response time of 20 ps, making black phosphorus a candidate for high performance THz detection at room temperature.

Tunable Ultrafast Thermal Relaxation in Graphene Measured by Continuous-Wave Photomixing.

Hot electron effects in graphene are significant because of graphene's small electronic heat capacity and weak electron-phonon coupling, yet the dynamics and cooling mechanisms of hot electrons in graphene are not completely understood. We describe a novel photocurrent spectroscopy method that uses the mixing of continuous-wave lasers in a graphene photothermal detector to measure the frequency dependence and nonlinearity of hot-electron cooling in graphene as a function of the carrier concentration and temperature. The method offers unparalleled sensitivity to the nonlinearity, and probes the ultrafast cooling of hot carriers with an optical fluence that is orders of magnitude smaller than in conventional time-domain methods, allowing for accurate characterization of electron-phonon cooling near charge neutrality. Our measurements reveal that near the charge neutral point the nonlinear power dependence of the electron cooling is dominated by disorder-assisted collisions, while at higher carrier concentrations conventional momentum-conserving cooling prevails in the nonlinear dependence. The relative contribution of these competing mechanisms can be electrostatically tuned through the application of a gate voltage-an effect that is unique to graphene.

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.

Pulsed Near-IR Photoresponse in a Bi-metal Contacted Graphene Photodetector.

We use an ultra-fast near-infrared pulse coincidence technique to study the time, temperature, and power dependence of the photoresponse of a bi-metal contacted graphene photodetector. We observe two components of the photovoltage signal. One component is gate-voltage dependent, linear in power at room temperature and sub-linear at low temperature-consistent with the hot-electron photothermoelectric effect due to absorption in the graphene. The power dependence is consistent with supercollision-dominated cooling in graphene. The other component is gate-voltage independent and linear in temperature and power, which we interpret as due to thermoelectricity of the metal electrodes due to differential light absorption.

Tunable Terahertz Hybrid Metal-Graphene Plasmons.

We report here a new type of plasmon resonance that occurs when graphene is connected to a metal. These new plasmon modes offer the potential to incorporate a tunable plasmonic channel into a device with electrical contacts, a critical step toward practical graphene terahertz optoelectronics. Through theory and experiments, we demonstrate, for example, anomalously high resonant absorption or transmission when subwavelength graphene-filled apertures are introduced into an otherwise conductive layer. These tunable plasmon resonances are essential yet missing ingredients needed for terahertz filters, oscillators, detectors, and modulators.

Plasmon-Enhanced Terahertz Photodetection in Graphene.

We report a large area terahertz detector utilizing a tunable plasmonic resonance in subwavelength graphene microribbons on SiC(0001) to increase the absorption efficiency. By tailoring the orientation of the graphene ribbons with respect to an array of subwavelength bimetallic electrodes, we achieve a condition in which the plasmonic mode can be efficiently excited by an incident wave polarized perpendicular to the electrode array, while the resulting photothermal voltage can be observed between the outermost electrodes.

Sensitive room-temperature terahertz detection via the photothermoelectric effect in graphene.

Terahertz radiation has uses in applications ranging from security to medicine. However, sensitive room-temperature detection of terahertz radiation is notoriously difficult. The hot-electron photothermoelectric effect in graphene is a promising detection mechanism; photoexcited carriers rapidly thermalize due to strong electron-electron interactions, but lose energy to the lattice more slowly. The electron temperature gradient drives electron diffusion, and asymmetry due to local gating or dissimilar contact metals produces a net current via the thermoelectric effect. Here, we demonstrate a graphene thermoelectric terahertz photodetector with sensitivity exceeding 10 V W(-1) (700 V W(-1)) at room temperature and noise-equivalent power less than 1,100 pW Hz(-1/2) (20 pW Hz(-1/2)), referenced to the incident (absorbed) power. This implies a performance that is competitive with the best room-temperature terahertz detectors for an optimally coupled device, and time-resolved measurements indicate that our graphene detector is eight to nine orders of magnitude faster than those. A simple model of the response, including contact asymmetries (resistance, work function and Fermi-energy pinning) reproduces the qualitative features of the data, and indicates that orders-of-magnitude sensitivity improvements are possible.

Approaching the limits of transparency and conductivity in graphitic materials through lithium intercalation.

Various band structure engineering methods have been studied to improve the performance of graphitic transparent conductors; however, none has demonstrated an increase of optical transmittance in the visible range. Here we measure in situ optical transmittance spectra and electrical transport properties of ultrathin graphite (3-60 graphene layers) simultaneously during electrochemical lithiation/delithiation. On intercalation, we observe an increase of both optical transmittance (up to twofold) and electrical conductivity (up to two orders of magnitude), strikingly different from other materials. Transmission as high as 91.7% with a sheet resistance of 3.0 Ω per square is achieved for 19-layer LiC6, which corresponds to a figure of merit σ(dc)/σ(opt) = 1,400, significantly higher than any other continuous transparent electrodes. The unconventional modification of ultrathin graphite optoelectronic properties is explained by the suppression of interband optical transitions and a small intraband Drude conductivity near the interband edge. Our techniques enable investigation of other aspects of intercalation in nanostructures.

Impact of interface roughness on the performance of broadband blackbody absorber based on dielectric-metal film multilayers.

We report on factors affecting the performance of a broadband, mid-IR absorber based on multiple, alternating dielectric / metal layers. In particular, we investigate the effect of interface roughness. Atomic layer deposition produces both a dramatic suppression of the interface roughness and a significant increase in the optical absorption as compared to devices fabricated using a conventional thermal evaporation source. Absorption characteristics greater than 80% across a 300 K black body spectrum are achieved. We demonstrate a further increase in this absorption via the inclusion of a patterned, porous anti-reflection layer.

Broadband and mid-infrared absorber based on dielectric-thin metal film multilayers.

We propose a periodic multilayer structure of dielectric and metal interlayers to achieve a near-perfect broadband absorber of mid-infrared radiation. We examine the influence of four factors on its performance: (1) the interlayer metal conductance, (2) the number of dielectric layers, (3) a nanopatterned antireflective layer, and (4) a reflective metallic bottom layer for backreflection. Absorption characteristics greater than 99% of the 300 K and 500 K blackbody spectra are found for the optimized structures. Incident angle and polarization dependence of the absorption spectra are examined. We also investigate the possibility of fabricating a nanopatterned antireflective layer to maximize absorption.

Suppression of long-range collective effects in meta-surfaces formed by plasmonic antenna pairs.

The collective effects in a periodic array of plasmonic double-antenna meta-molecules are studied. We experimentally observe that the collective behavior in this structure substantially differs from the one observed in their single-antenna counterparts. This behavior is explained using an analytical dipole model. We find that in the double-antenna case the effective dipole-dipole interaction is significantly modified and the transverse long-range interaction is suppressed, giving rise to the disappearance of Wood's anomalies. Numerical calculations also show that such suppression of long-range interaction results in an anomalous spatial dispersion of the electric-dipolar mode, making it insensitive to the angle of incidence. In contrast, the quadrupolar mode of the antenna pair experiences strong spatial dispersion. These results show that collective effects in plasmonic metamaterials are very sensitive to the design and topology of meta-molecules. Our findings envision the possibility of suppressing the spatial dispersion effects to weaken the dependence of the metamaterials' response on the incidence angle.

Topological quantization in units of the fine structure constant.

Fundamental topological phenomena in condensed matter physics are associated with a quantized electromagnetic response in units of fundamental constants. Recently, it has been predicted theoretically that the time-reversal invariant topological insulator in three dimensions exhibits a topological magnetoelectric effect quantized in units of the fine structure constant α=e²/ℏc. In this Letter, we propose an optical experiment to directly measure this topological quantization phenomenon, independent of material details. Our proposal also provides a way to measure the half-quantized Hall conductances on the two surfaces of the topological insulator independently of each other.

Near-field evidence for ferromagnetic "nanoneedles" in Nd1/2Sr1/2MnO3.

We report on the near-field optical microscopic (NSOM) imaging of single-crystal Nd1/2Sr1/2MnO3 near the first-order phase transition from the CE-type charge-ordered insulator (COI) to the ferromagnetic metal (FMM) at 165 K. Using polarized light, the measurements are sensitive to twin domains through optical anisotropy and to hysteretic inhomogeneous strain associated with the phase transition. Optical evidence for strain relaxation and multiphase coexistence is observed through the transition from 150 to 165 K. The multiphase coexistence is seen as the formation of FMM "nanoneedles" with widths less than 100 nm and lengths of at least several micrometers at temperatures well below TC. The work demonstrates polarized NSOM as a technique for the study of first-order solid-state phase transformations on the nanometer spatial scale.

Development of high-throughput, polarization-maintaining, near-field probes.

A novel, chemical-etching technique produces very high throughput, polarization-maintaining probes for near-field, scanning, optical microscopy (NSOM). The process includes coating the tips with aluminum and forming the apertures with a focused ion beam (FIB). The elliptical core fibers used resulted in elliptical apertures for the probes. The throughput of the probes depends on the incident polarization. For polarization parallel to the minor axis, the tip presents an insertion loss of only 20 dB for aperture widths of 55 nm. Probes have a typical polarization extinction of 100 to 1 in the far field. These tips produced NSOM images of gold dots on a GaAs substrate in reflection mode.