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 Broadband Nanocarbon Transparent Conductor by Electrochemical Intercalation.

Optical transparent and electrical conducting materials with broadband transmission are important for many applications in optoelectronic, telecommunications, and military devices. However, studies of broadband transparent conductors and their controlled modulation are scarce. In this study, we report that reversible transmittance modulation has been achieved with sandwiched nanocarbon thin films (containing carbon nanotubes (CNTs) and reduced graphene oxide (rGO)) via electrochemical alkali-ion intercalation/deintercalation. The transmittance modulation covers a broad range from the visible (450 nm) to the infrared (5 µm), which can be achieved only by rGO rather than pristine graphene films. The large broadband transmittance modulation is understood with DFT calculations, which suggest a decrease in interband transitions in the visible range as well as a reduced reflection in the IR range upon intercalation. We find that a larger interlayer distance in few-layer rGO results in a significant increase in transparency in the infrared region of the spectrum, in agreement with experimental results. Furthermore, a reduced plasma frequency in rGO compared to few-layer graphene is also important to understand the experimental results for broadband transparency in rGO. The broadband transmittance modulation of the CNT/rGO/CNT systems can potentially lead to electrochromic and thermal camouflage applications.

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.

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.

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.

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.