Light-driven nanoscale vectorial currents.

Controlled charge flows are fundamental to many areas of science and technology, serving as carriers of energy and information, as probes of material properties and dynamics1 and as a means of revealing2,3 or even inducing4,5 broken symmetries. Emerging methods for light-based current control5-16 offer particularly promising routes beyond the speed and adaptability limitations of conventional voltage-driven systems. However, optical generation and manipulation of currents at nanometre spatial scales remains a basic challenge and a crucial step towards scalable optoelectronic systems for microelectronics and information science. Here we introduce vectorial optoelectronic metasurfaces in which ultrafast light pulses induce local directional charge flows around symmetry-broken plasmonic nanostructures, with tunable responses and arbitrary patterning down to subdiffractive nanometre scales. Local symmetries and vectorial currents are revealed by polarization-dependent and wavelength-sensitive electrical readout and terahertz (THz) emission, whereas spatially tailored global currents are demonstrated in the direct generation of elusive broadband THz vector beams17. We show that, in graphene, a detailed interplay between electrodynamic, thermodynamic and hydrodynamic degrees of freedom gives rise to rapidly evolving nanoscale driving forces and charge flows under the extremely spatially and temporally localized excitation. These results set the stage for versatile patterning and optical control over nanoscale currents in materials diagnostics, THz spectroscopies, nanomagnetism and ultrafast information processing.

Broadband Linear-to-Circular Polarization Conversion Enabled by Birefringent Off-Resonance Reflective Metasurfaces.

Due to the scarcity of circular polarization light sources, linear-to-circular polarization conversion is required to generate circularly polarized light for a variety of applications. Despite significant past efforts, broadband linear-to-circular polarization conversion remains elusive particularly in the terahertz and midinfrared frequency ranges. Here we propose a novel mechanism based on coupled mode theory, and experimentally demonstrate at terahertz frequencies that highly efficient (power conversion efficiency approaching unity) and ultrabroadband (fractional bandwidth up to 80%) linear-to-circular polarization conversion can be accomplished by the judicious design of birefringent metasurfaces. The underlying mechanism operates in the frequency range between well separated resonances, and relies upon the phase response of these resonances away from the resonant frequencies, as well as the balance of the resonant and nonresonant channels. This mechanism is applicable for any operating frequencies from microwave to visible. The present Letter potentially opens a wide range of opportunities in wireless communications, spectroscopy, and emergent quantum materials research where circularly polarized light is desired.

High-Temperature Refractory Metasurfaces for Solar Thermophotovoltaic Energy Harvesting.

Solar energy promises a viable solution to meet the ever-increasing power demand by providing a clean, renewable energy alternative to fossil fuels. For solar thermophotovoltaics (STPV), high-temperature absorbers and emitters with strong spectral selectivity are imperative to efficiently couple solar radiation into photovoltaic cells. Here, we demonstrate refractory metasurfaces for STPV with tailored absorptance and emittance characterized by in situ high-temperature measurements, featuring thermal stability up to at least 1200 °C. Our tungsten-based metasurface absorbers have close-to-unity absorption from visible to near-infrared and strongly suppressed emission at longer wavelengths, while our metasurface emitters provide wavelength-selective emission spectrally matched to the band-edge of InGaAsSb photovoltaic cells. The projected overall STPV efficiency is as high as 18% when a fully integrated absorber/emitter metasurface structure is employed, which is comparable to the efficiencies of the best currently available commercial single-junction PV cells and can be further improved to potentially exceed those in mainstream photovoltaic technologies. Our work opens a path forward for high-performance STPV systems based on refractory metasurface structures.

Conducting Interface in Oxide Homojunction: Understanding of Superior Properties in Black TiO2.

Black TiO2 nanoparticles with a crystalline core and amorphous-shell structure exhibit superior optoelectronic properties in comparison with pristine TiO2. The fundamental mechanisms underlying these enhancements, however, remain unclear, largely due to the inherent complexities and limitations of powder materials. Here, we fabricate TiO2 homojunction films consisting of an oxygen-deficient amorphous layer on top of a highly crystalline layer, to simulate the structural/functional configuration of black TiO2 nanoparticles. Metallic conduction is achieved at the crystalline-amorphous homointerface via electronic interface reconstruction, which we show to be the main reason for the enhanced electron transport of black TiO2. This work not only achieves an unprecedented understanding of black TiO2 but also provides a new perspective for investigating carrier generation and transport behavior at oxide interfaces, which are of tremendous fundamental and technological interest.

A review of metasurfaces: physics and applications.

Metamaterials are composed of periodic subwavelength metal/dielectric structures that resonantly couple to the electric and/or magnetic components of the incident electromagnetic fields, exhibiting properties that are not found in nature. This class of micro- and nano-structured artificial media have attracted great interest during the past 15 years and yielded ground-breaking electromagnetic and photonic phenomena. However, the high losses and strong dispersion associated with the resonant responses and the use of metallic structures, as well as the difficulty in fabricating the micro- and nanoscale 3D structures, have hindered practical applications of metamaterials. Planar metamaterials with subwavelength thickness, or metasurfaces, consisting of single-layer or few-layer stacks of planar structures, can be readily fabricated using lithography and nanoprinting methods, and the ultrathin thickness in the wave propagation direction can greatly suppress the undesirable losses. Metasurfaces enable a spatially varying optical response (e.g. scattering amplitude, phase, and polarization), mold optical wavefronts into shapes that can be designed at will, and facilitate the integration of functional materials to accomplish active control and greatly enhanced nonlinear response. This paper reviews recent progress in the physics of metasurfaces operating at wavelengths ranging from microwave to visible. We provide an overview of key metasurface concepts such as anomalous reflection and refraction, and introduce metasurfaces based on the Pancharatnam-Berry phase and Huygens' metasurfaces, as well as their use in wavefront shaping and beam forming applications, followed by a discussion of polarization conversion in few-layer metasurfaces and their related properties. An overview of dielectric metasurfaces reveals their ability to realize unique functionalities coupled with Mie resonances and their low ohmic losses. We also describe metasurfaces for wave guidance and radiation control, as well as active and nonlinear metasurfaces. Finally, we conclude by providing our opinions of opportunities and challenges in this rapidly developing research field.

Excitation of dark plasmonic modes in symmetry broken terahertz metamaterials.

Plasmonic structures with high symmetry, such as double-identical gap split ring resonators, possess dark eigenmodes. These dark eigenmodes are dominated by magnetic dipole and/or higher-order multi-poles such as electric quadrapoles. Consequently these dark modes interact very weakly with the surrounding environment, and can have very high quality factors (Q). In this work, we have studied, experimentally as well as theoretically, these dark eigenmodes in terahertz metamaterials. Theoretical investigations with the help of classical perturbation theory clearly indicate the existence of these dark modes in symmetric plasmonic metamaterials. However, these dark modes can be excited experimentally by breaking the symmetry within the constituting metamaterial resonators cell, resulting in high quality factor resonance mode. The symmetry broken metamaterials with such high quality factor can pave the way in realizing high sensitivity sensors, in addition to other applications.

Ultrafast terahertz emission from emerging symmetry-broken materials.

Nonlinear optical spectroscopies are powerful tools for investigating both static material properties and light-induced dynamics. Terahertz (THz) emission spectroscopy has emerged in the past several decades as a versatile method for directly tracking the ultrafast evolution of physical properties, quasiparticle distributions, and order parameters within bulk materials and nanoscale interfaces. Ultrafast optically-induced THz radiation is often analyzed mechanistically in terms of relative contributions from nonlinear polarization, magnetization, and various transient free charge currents. While this offers material-specific insights, more fundamental symmetry considerations enable the generalization of measured nonlinear tensors to much broader classes of systems. We thus frame the present discussion in terms of underlying broken symmetries, which enable THz emission by defining a system directionality in space and/or time, as well as more detailed point group symmetries that determine the nonlinear response tensors. Within this framework, we survey a selection of recent studies that utilize THz emission spectroscopy to uncover basic properties and complex behaviors of emerging materials, including strongly correlated, magnetic, multiferroic, and topological systems. We then turn to low-dimensional systems to explore the role of designer nanoscale structuring and corresponding symmetries that enable or enhance THz emission. This serves as a promising route for probing nanoscale physics and ultrafast light-matter interactions, as well as facilitating advances in integrated THz systems. Furthermore, the interplay between intrinsic and extrinsic material symmetries, in addition to hybrid structuring, may stimulate the discovery of exotic properties and phenomena beyond existing material paradigms.

Low-loss ultra-high-Q dark mode plasmonic Fano metamaterials.

We experimentally demonstrate a planar terahertz Fano metamaterial with an ultrahigh quality (Q) factor of 227. This is achieved by the excitation of the nonradiative dark modes by introducing a tiny asymmetry in the metamaterial structure. The extremely sharp quadrupole and Fano resonances are excited at normal incidence for orthogonal polarizations of the electric field. In order to capture the narrow linewidth of the dark resonance modes, we perform high resolution terahertz time-domain measurements with a scan length of 200 picoseconds and frequency resolution of 5 GHz. These high-Q metamaterials can be used in ultrasensitive label-free terahertz sensing, dense photonic integration, and narrowband filtering.

Experimental demonstration of terahertz metamaterial absorbers with a broad and flat high absorption band.

We present the design, numerical simulations and experimental measurements of terahertz metamaterial absorbers with a broad and flat absorption top over a wide incidence angle range for either transverse electric or transverse magnetic polarization depending on the incident direction. The metamaterial absorber unit cell consists of two sets of structures resonating at different but close frequencies. The overall absorption spectrum is the superposition of individual components and becomes flat at the top over a significant bandwidth. The experimental results are in excellent agreement with numerical simulations.

Active terahertz metamaterial devices.

The development of artificially structured electromagnetic materials, termed metamaterials, has led to the realization of phenomena that cannot be obtained with natural materials. This is especially important for the technologically relevant terahertz (1 THz = 10(12) Hz) frequency regime; many materials inherently do not respond to THz radiation, and the tools that are necessary to construct devices operating within this range-sources, lenses, switches, modulators and detectors-largely do not exist. Considerable efforts are underway to fill this 'THz gap' in view of the useful potential applications of THz radiation. Moderate progress has been made in THz generation and detection; THz quantum cascade lasers are a recent example. However, techniques to control and manipulate THz waves are lagging behind. Here we demonstrate an active metamaterial device capable of efficient real-time control and manipulation of THz radiation. The device consists of an array of gold electric resonator elements (the metamaterial) fabricated on a semiconductor substrate. The metamaterial array and substrate together effectively form a Schottky diode, which enables modulation of THz transmission by 50 per cent, an order of magnitude improvement over existing devices.

Tailored resonator coupling for modifying the terahertz metamaterial response.

We experimentally and numerically study the nature of coupling between laterally paired terahertz metamaterial split-ring resonators. Coupling is shown to modify the inductive-capacitive (LC) resonances resulting in either red or blue-shifting. Results indicate that tuning of the electric and magnetic coupling parameters may be accomplished not by changing the orientation or density of SRRs, but by a design modification at the unit cell level. These experiments illustrate additional degrees of freedom in tuning the electromagnetic response, which offers a path to more robust metamaterial designs.

Ultrafast nonlinear optical spectroscopy of a dual-band negative index metamaterial all-optical switching device.

We study the nonlinear optical response of a fishnet structure-metamaterial all-optical switching device that exhibits two near-infrared negative-index resonances. We study and compare the nonlinear optical response at both resonances and identify transient spectral features associated with the negative index resonance. We see a significantly stronger response at the longer wavelength resonance, but identical temporal dynamics at both resonances, providing insight into separately engineering the switching time and switching ratio of such a fishnet structure metamaterial all-optical switch. We also numerically reproduce the nonlinear behavior of our device using the Drude conductivity model and a finite integration technique over wide spectral and pump fluence ranges. Thereby, we show that beyond the linear properties of the device, the magnitude of the pump-probe response is completely described by only two material parameters. These results provide insight into engineering various aspects of the nonlinear response of fishnet structure metamaterials.

A broadband planar terahertz metamaterial with nested structure.

We demonstrate the broadening of fundamental resonance in terahertz metamaterial by successive insertion of metal rings in the original unit cell of a split ring resonator (SRR) forming an inter connected nested structure. With the subsequent addition of each inner ring, the fundamental resonance mode shows gradual broadening and blue shift. For a total of four rings in the structure the resonance linewidth is enhanced by a factor of four and the blue shift is as large as 316 GHz. The dramatic increase in fundamental resonance broadening and its blue shifting is attributed to the decrease in the effective inductance of the entire SRR structure with addition of each smaller ring. We also observe that while the fundamental resonance is well preserved, the dipolar mode resonance undergoes multiple splittings with the addition of each ring in the nest. Such planar metamaterials, possessing broadband resonant response in the fundamental mode of operation, could have potential applications for extending the properties of metamaterials over a broader frequency range of operations.

Thermal tunability in terahertz metamaterials fabricated on strontium titanate single-crystal substrates.

We report an experimental demonstration of thermal tuning of resonance frequency in a planar terahertz metamaterial consisting of a gold split-ring resonator array fabricated on a bulk single-crystal strontium titanate (SrTiO3) substrate. Cooling the metamaterial starting from 409 K down to 150 K causes about a 43% shift in resonance frequency, and there is very little variation in resonance strength. The resonance shift is due to the temperature-dependent dielectric constant of the strontium titanate. The experiment opens up avenues for designing tunable terahertz devices by exploiting the temperature-sensitive characteristic of high dielectric constant substrates and complex metal oxide materials.

Ultrafast hopping dynamics of 5f electrons in the Mott insulator UO2 studied by femtosecond pump-probe spectroscopy.

We describe a femtosecond pump-probe study of ultrafast hopping dynamics of 5f electrons in the Mott insulator UO2 following Mott-gap excitation at temperatures of 5-300 K. Hopping-induced response of the lattice and electrons is probed by transient reflectivity at mid- and above-gap photon energies, respectively. These measurements show an instantaneous hop, subsequent picosecond lattice deformation, followed by acoustic phonon emission and microsecond relaxation. Temperature-dependent studies indicate that the slow relaxation results from Hubbard excitons formed by U³âº-U5⁺ pairs.

Orientation dependent far-infrared terahertz absorptions in single crystal pentaerythritol tetranitrate (PETN) using terahertz time-domain spectroscopy.

Terahertz time-domain spectroscopy (THZ-TDS) has been used to measure the absorption spectra in the range 7-100 cm(-1) (0.2-3 THz) of single crystal pentaerythritol tetranitrate (PETN). Absorption was measured in transmission mode as a function of incident polarization with the incident and transmitted wave vectors oriented along the crystallographic directions [100], <10(a/c)(2)>, and <110>. Samples were rotated with respect to the incident polarization while absorption was measured at both 300 and 20 K. Comparatively minor differences were observed among the three orientations. Two broad absorptions at 72 and >90 cm(-1), and several weaker absorptions at 36, 55, 80, and 82 cm(-1), have been observed at cryogenic temperatures.

Diabolical point and conical-like diffraction in periodic plasmonic nanostructures.

We present the formation of a singular (diabolical) point in k-space from a periodic metal-dielectric waveguide array. The singularity originates from the balance between alternating normal and anomalous coupling. We numerically demonstrate a strong diffraction anomaly (conical-like diffraction) near the singular point. We also show the evolution of the diffraction pattern with band deformation. The resultant peculiar propagation dynamics of surface plasmon polaritons could provide a new toolset for manipulating light on the nano-scale.

Dirac dynamics in one-dimensional graphene-like plasmonic crystals: pseudo-spin, chirality, and diffraction anomaly.

We introduce a new class of plasmonic crystals possessing graphene-like internal symmetries and Dirac-type spectrum in k-space. We study dynamics of surface plasmon polaritons supported in the plasmonic crystals by employing the formalism of Dirac dynamics for relativistic quantum particles. Through an analogy with graphene, we introduce a concept of pseudo-spin and chirality to indicate built-in symmetry of the plasmonic crystals near Dirac point. The surface plasmon polaritons with different pseudo-spin states are shown to split in the crystals into two beams, analogous to spin Hall effect.

Large dynamic resonance transition between surface plasmon and localized surface plasmon modes.

We present resonant terahertz transmission in a composite plasmonic film comprised of an array of subwavelength metallic patches and semiconductor holes. A large dynamic transition between a dipolar localized surface plasmon mode and a surface plasmon resonance near 0.8 THz is observed under near infrared optical excitation. The reversal in transmission amplitude from a stop-band to a pass-band and up to pi/2 phase shift achieved in the composite plasmonic film make it promising in large dynamic phase modulation, optical changeover switching, and active terahertz plasmonics.

Antireflection coating using metamaterials and identification of its mechanism.

We present a novel approach of antireflection coating using metamaterials. It dramatically reduces the reflection and greatly enhances the transmission near a specifically designed frequency over a wide range of incidence angles for both transverse magnetic and transverse electric polarizations. A classical interference mechanism is identified through analytical derivations and numerical simulations. It elucidates that the tailored magnitude and phase of waves reflected and transmitted at boundaries of metamaterial coating are responsible for the antireflection.