Shcherbakov, Maxim R.; Liu, Sheng L.; Zubyuk, Varvara V.; Vaskin, Aleksandr; Vabishchevich, Polina P.; Keeler, Gordon A.; Pertsch, Thomas; Dolgova, Tatyana V.; Staude, Isabelle; Brener, Igal B.; Fedyanin, Andrey A.
Optical metasurfaces are regular quasi-planar nanopatterns that can apply diverse spatial and spectral transformations to light waves. However, metasurfaces are no longer adjustable after fabrication, and a critical challenge is to realise a technique of tuning their optical properties that is both fast and efficient. We experimentally realise an ultrafast tunable metasurface consisting of subwavelength gallium arsenide nanoparticles supporting Mie-type resonances in the near infrared. Using transient reflectance spectroscopy, we demonstrate a picosecond-scale absolute reflectance modulation of up to 0.35 at the magnetic dipole resonance of the metasurfaces and a spectral shift of the resonance by 30 nm, both achieved at unprecedentedly low pump fluences of less than 400 μJ cm-2. Our findings thereby enable a versatile tool for ultrafast and efficient control of light using light.
We experimentally demonstrate resonantly enhanced nonlinear optical processes such as 2nd-, 3rd-, and 4th-harmonic generations, sum-frequency generation, four-wave mixing processes, etc., in the visible and near-IR using GaAs dielectric metasurfaces.
We demonstrate the active tuning of all-dielectric metasurfaces exhibiting high-quality factor (high-Q) resonances. The active control is provided by embedding the asymmetric silicon meta-atoms with liquid crystals, which allows the relative index of refraction to be controlled through heating. It is found that high quality factor resonances (Q = 270 ± 30) can be tuned over more than three resonance widths. Our results demonstrate the feasibility of using all-dielectric metasurfaces to construct tunable narrow-band filters.
Dielectric metasurfaces that exploit the different Mie resonances of nanoscale dielectric resonators are a powerful platform for manipulating electromagnetic fields and can provide novel optical behavior. In this work, we experimentally demonstrate independent tuning of the magnetic dipole resonances relative to the electric dipole resonances of split dielectric resonators (SDRs). By increasing the split dimension, we observe a blue shift of the magnetic dipole resonance toward the electric dipole resonance. Therefore, SDRs provide the ability to directly control the interaction between the two dipole resonances within the same resonator. For example, we achieve the first Kerker condition by spectrally overlapping the electric and magnetic dipole resonances and observe significantly suppressed backward scattering. Moreover, we show that a single SDR can be used as an optical nanoantenna that provides strong unidirectional emission from an electric dipole source.
We experimentally demonstrate ultrahigh extinction ratio (>65 dB) amplitude modulators (AMs) that can be electrically tuned to operate across a broad spectral range of 160 nm from 1480-1640 nm and 95 nm from 1280-1375 nm. Our on-chip AMs employ one extra coupler compared with conventional Mach-Zehnder interferometers (MZI), thus form a cascaded MZI (CMZI) structure. Either directional or adiabatic couplers are used to compose the CMZI AMs and experimental comparisons are made between these two different structures. We investigate the performance of CMZI AMs under extreme conditions such as using 95:5 split ratio couplers and unbalanced waveguide losses. Electro-optic phase shifters are also integrated in the CMZI AMs for high-speed operation. Finally, we investigate the output optical phase when the amplitude is modulated, which provides us valuable information when both amplitude and phase are to be controlled. Our demonstration not only paves the road to applications such as quantum information processing that requires high extinction ratio AMs but also significantly alleviates the tight fabrication tolerance needed for large-scale integrated photonics.
We report lasing from nonpolar p-i-n InGaN/GaN multi-quantum well core-shell single-nanowire lasers by optical pumping at room temperature. The nanowire lasers were fabricated using a hybrid approach consisting of a top-down two-step etch process followed by a bottom-up regrowth process, enabling precise geometrical control and high material gain and optical confinement. The modal gain spectra and the gain curves of the core-shell nanowire lasers were measured using micro-photoluminescence and analyzed using the Hakki-Paoli method. Significantly lower lasing thresholds due to high optical gain were measured compared to previously reported semipolar InGaN/GaN core-shell nanowires, despite significantly shorter cavity lengths and reduced active region volume. Mode simulations show that due to the core-shell architecture, annular-shaped modes have higher optical confinement than solid transverse modes. The results show the viability of this p-i-n nonpolar core-shell nanowire architecture, previously investigated for next-generation light-emitting diodes, as low-threshold, coherent UV-visible nanoscale light emitters, and open a route toward monolithic, integrable, electrically injected single-nanowire lasers operating at room temperature.
We demonstrate the ultrafast formation of terahertz (THz) metasurfaces through all-optical creation of spatially modulated carrier density profiles in a deep-subwavelength GaAs film. The switch-on of the transient plasmon mode, governed by the GaAs effective electron mass and electron− phonon interactions, is revealed by structured-optical pump THz probe spectroscopy, on a time scale of 500 fs. By modulating the carrier density using different pump fluences, we observe a wide tuning of the electric dipole resonance of the transient GaAs metasurface from 0.5 THz to 1.7 THz. Furthermore, we numerically demonstrate that the metasurface presented here can be generalized to more complex architectures for realizing functionalities such as perfect absorption, leading to a 30 dB modulation depth. The platform also provides a pathway to achieve ultrafast manipulation of infrared beams in the linear and, potentially, nonlinear regime.
We experimentally demonstrate amplitude modulators (AMs) with >65 dB extinction across over a 160 nm spectral range. The output optical phase response is also characterized when the amplitude is modulated.
We present a new approach to dielectric metasurface design that relies on a single resonator per unit cell and produces robust, high quality factor Fano resonances. Our approach utilizes symmetry breaking of highly symmetric resonator geometries, such as cubes, to induce couplings between the otherwise orthogonal resonator modes. In particular, we design perturbations that couple "bright" dipole modes to "dark" dipole modes whose radiative decay is suppressed by local field effects in the array. Our approach is widely scalable from the near-infrared to radio frequencies. We first unravel the Fano resonance behavior through numerical simulations of a germanium resonator-based metasurface that achieves a quality factor of ∼1300 at ∼10.8 μm. Then, we present two experimental demonstrations operating in the near-infrared (∼1 μm): a silicon-based implementation that achieves a quality factor of ∼350; and a gallium arsenide-based structure that achieves a quality factor of ∼600, the highest near-infrared quality factor experimentally demonstrated to date with this kind of metasurface. Importantly, large electromagnetic field enhancements appear within the resonators at the Fano resonant frequencies. We envision that combining high quality factor, high field enhancement resonances with nonlinear and active/gain materials such as gallium arsenide will lead to new classes of active optical devices.
We present all-dielectric 2D and 3D metamaterials that are monolithically fabricated from III-V semiconductor nanostructures. The active/gain and high optical nonlinearity properties of the metamaterials can lead to new classes of active devices.
We experimentally observe large enhancement of second-harmonic generation (SHG) from GaAs metasurfaces. The SHG polarization when excited at the electric and magnetic dipole resonances is orthogonal and can be attributed to different nonlinear generation mechanisms.
Metamaterial dielectric resonators represent a promising path toward low-loss metamaterials at optical frequencies. In this paper we utilize perturbations of high symmetry resonator geometries, such as cubes, either to overlap the electric and magnetic dipole resonances, thereby enabling directional scattering and Huygens' metasurfaces, or to induce couplings between the otherwise orthogonal resonator modes to achieve high-quality factor Fano resonances. Our results are fully scalable across any frequency bands where high-permittivity dielectric materials are available, including microwave, THz, and infrared frequencies.
Nonlinear optical phenomena in nanostructured materials have been challenging our perceptions of nonlinear optical processes that have been explored since the invention of lasers. For example, the ability to control optical field confinement, enhancement, and scattering almost independently allows nonlinear frequency conversion efficiencies to be enhanced by many orders of magnitude compared to bulk materials. Also, the subwavelength length scale renders phase matching issues irrelevant. Compared with plasmonic nanostructures, dielectric resonator metamaterials show great promise for enhanced nonlinear optical processes due to their larger mode volumes. Here, we present, for the first time, resonantly enhanced second-harmonic generation (SHG) using gallium arsenide (GaAs) based dielectric metasurfaces. Using arrays of cylindrical resonators we observe SHG enhancement factors as large as 104 relative to unpatterned GaAs. At the magnetic dipole resonance, we measure an absolute nonlinear conversion efficiency of ∼2 × 10-5 with ∼3.4 GW/cm2 pump intensity. The polarization properties of the SHG reveal that both bulk and surface nonlinearities play important roles in the observed nonlinear process.
We demonstrate intrinsic, linearly polarized lasing from single GaN nanowires using cross-sectional shape control. A two-step top-down fabrication approach was employed to create straight nanowires with controllable rectangular cross-sections. A clear lasing threshold of 444 kW cm-2 and a narrow spectral line width of 0.16 nm were observed under optical pumping at room temperature, indicating the onset of lasing. The polarization was along the short dimension (y-direction) of the nanowire due to the higher transverse confinement factors for y-polarized transverse modes resulting from the rectangular nanowire cross-section. The results show that cross-sectioned shape control can enable inherent control over the polarization of nanowire lasers without additional environment requirements, such as placement onto lossy substrates.
Subwavelength-thin metasurfaces have shown great promises for the control of optical wavefronts, thus opening new pathways for the development of efficient flat optics. In particular, Huygens’ metasurfaces based on all-dielectric resonant meta-atoms have already shown a huge potential for practical applications with their polarization insensitivity and high transmittance efficiency. Here, we experimentally demonstrate a holographic Huygens’ metasurface based on dielectric resonant meta-atoms capable of complex wavefront control at telecom wavelengths. Our metasurface produces a hologram image in the far-field with 82% transmittance efficiency and 40% imaging efficiency. Such efficient complex wavefront control shows that Huygens’ metasurfaces based on resonant dielectric meta-atoms are a big step towards practical applications of metasurfaces in wavefront design related technologies, including computer-generated holograms, ultra-thin optics, security and data storage devices.
Epsilon-near-zero (ENZ) modes arising from condensed-matter excitations such as phonons and plasmons are a new path for tailoring light-matter interactions at the nanoscale. Complex spectral shaping can be achieved by creating such modes in nanoscale semiconductor layers and controlling their interaction with multiple, distinct, dipole resonant systems. Examples of this behavior are presented at midinfrared frequencies for ENZ modes that are strongly coupled to metamaterial resonators and simultaneously strongly coupled to semiconductor phonons or quantum-well intersubband transitions (ISTs), resulting in double- and triple-polariton branches in transmission spectra. For the double-polariton branch case, we find that the best strategy to maximize the Rabi splitting is to use a combination of a doped layer supporting an ENZ feature and a layer supporting ISTs, with overlapping ENZ and IST frequencies. This design flexibility renders this platform attractive for low-voltage tunable filters, light-emitting diodes, and efficient nonlinear composite materials.
Establishing processing-structure-property relationships for monolayer materials is crucial for a range of applications spanning optics, catalysis, electronics and energy. Presently, for molybdenum disulfide, a promising catalyst for artificial photosynthesis, considerable debate surrounds the structure/property relationships of its various allotropes. Here we unambiguously solve the structure of molybdenum disulfide monolayers using high-resolution transmission electron microscopy supported by density functional theory and show lithium intercalation to direct a preferential transformation of the basal plane from 2H (trigonal prismatic) to 1T′ (clustered Mo). These changes alter the energetics of molybdenum disulfide interactions with hydrogen (ΔG H), and, with respect to catalysis, the 1T′ transformation renders the normally inert basal plane amenable towards hydrogen adsorption and hydrogen evolution. Indeed, we show basal plane activation of 1T′ molybdenum disulfide and a lowering of ΔG H from +1.6 eV for 2H to +0.18 eV for 1T′, comparable to 2H molybdenum disulfide edges on Au(111), one of the most active hydrogen evolution catalysts known.
QD-solids comprising self-assembled semiconductor nanocrystals such as CdSe are currently under investigation for use in a wide array of applications including light emitting diodes, solar cells, field effect transistors, photodetectors, and biosensors. The goal of this LDRD project was develop a fundamental understanding of the relationship between nanoparticle interactions and the different regimes of charge and energy transport in semiconductor quantum dot (QD) solids. Interparticle spacing was tuned through the application of hydrostatic pressure in a diamond anvil cell, and the impact on interparticle interactions was probed using x-ray scattering and a variety of static and transient optical spectroscopies. During the course of this LDRD, we discovered a new, previously unknown, route to synthesize semiconductor quantum wires using high pressure sintering of self-assembled quantum dot crystals. We believe that this new, pressure driven synthesis approach holds great potential as a new tool for nanomaterials synthesis and engineering.
There is strong interest in minimizing the volume of lasers to enable ultracompact, low-power, coherent light sources. Nanowires represent an ideal candidate for such nanolasers as stand-alone optical cavities and gain media, and optically pumped nanowire lasing has been demonstrated in several semiconductor systems. Electrically injected nanowire lasers are needed to realize actual working devices but have been elusive due to limitations of current methods to address the requirement for nanowire device heterostructures with high material quality, controlled doping and geometry, low optical loss, and efficient carrier injection. In this project we proposed to demonstrate electrically injected single nanowire lasers emitting in the important UV to visible wavelengths. Our approach to simultaneously address these challenges is based on high quality III-nitride nanowire device heterostructures with precisely controlled geometries and strong gain and mode confinement to minimize lasing thresholds, enabled by a unique top-down nanowire fabrication technique.
We experimentally demonstrate a functional silicon metadevice at telecom wavelengths that can efficiently control the wavefront of optical beams by imprinting a spatially varying transmittance phase independent of the polarization of the incident beam. Near-unity transmittance efficiency and close to 0-2 phase coverage are enabled by utilizing the localized electric and magnetic Mie-type resonances of low-loss silicon nanoparticles tailored to behave as electromagnetically dual-symmetric scatterers. We apply this concept to realize a metadevice that converts a Gaussian beam into a vortex beam. The required spatial distribution of transmittance phases is achieved by a variation of the lattice spacing as a single geometric control parameter.
Coherent superposition of light from subwavelength sources is an attractive prospect for the manipulation of the direction, shape and polarization of optical beams. This phenomenon constitutes the basis of phased arrays, commonly used at microwave and radio frequencies. Here we propose a new concept for phased-array sources at infrared frequencies based on metamaterial nanocavities coupled to a highly nonlinear semiconductor heterostructure. Optical pumping of the nanocavity induces a localized, phase-locked, nonlinear resonant polarization that acts as a source feed for a higher-order resonance of the nanocavity. Varying the nanocavity design enables the production of beams with arbitrary shape and polarization. As an example, we demonstrate two second harmonic phased-array sources that perform two optical functions at the second harmonic wavelength (∼5μm): a beam splitter and a polarizing beam splitter. Proper design of the nanocavity and nonlinear heterostructure will enable such phased arrays to span most of the infrared spectrum.
We report continuous, dynamic, reversible, and widely tunable lasing from 367 to 337 nm from single GaN nanowires (NWs) by applying hydrostatic pressure up to ∼7 GPa. The GaN NW lasers, with heights of 4-5 μm and diameters ∼140 nm, are fabricated using a lithographically defined two-step top-down technique. The wavelength tuning is caused by an increasing Γ direct bandgap of GaN with increasing pressure and is precisely controllable to subnanometer resolution. The observed pressure coefficients of the NWs are ∼40% larger compared with GaN microstructures fabricated from the same material or from reported bulk GaN values, revealing a nanoscale-related effect that significantly enhances the tuning range using this approach. This approach can be generally applied to other semiconductor NW lasers to potentially achieve full spectral coverage from the UV to IR.
We experimentally demonstrate efficient third harmonic generation from an indium tin oxide nanofilm (λ/42 thick) on a glass substrate for a pump wavelength of 1.4 μm. A conversion efficiency of 3.3 × 10-6 is achieved by exploiting the field enhancement properties of the epsilon-near-zero mode with an enhancement factor of 200. This nanoscale frequency conversion method is applicable to other plasmonic materials and reststrahlen materials in proximity of the longitudinal optical phonon frequencies.
We employ both the effective medium approximation (EMA) and Bloch theory to compare the dispersion properties of semiconductor hyperbolic metamaterials (SHMs) at mid-infrared frequencies and metallic hyperbolic metamaterials (MHMs) at visible frequencies. This analysis reveals the conditions under which the EMA can be safely applied for both MHMs and SHMs. We find that the combination of precise nanoscale layering and the longer infrared operating wavelengths puts the SHMs well within the effective medium limit and, in contrast to MHMs, allows for the attainment of very high photon momentum states. In addition, SHMs allow for new phenomena such as ultrafast creation of the hyperbolic manifold through optical pumping. In particular, we examine the possibility of achieving ultrafast topological transitions through optical pumping which can photo-dope appropriately designed quantum wells on the femtosecond time scale.
Lasing is demonstrated from gallium nitride nanotubes fabricated using a two-step top-down technique. By optically pumping, we observed characteristics of lasing: a clear threshold, a narrow spectral, and guided emission from the nanotubes. In addition, annular lasing emission from the GaN nanotube is also observed, indicating that cross-sectional shape control can be employed to manipulate the properties of nanolasers. The nanotube lasers could be of interest for optical nanofluidic applications or application benefitting from a hollow beam shape.
Ultrafast optical excitation of photocarriers has the potential to transform undoped semiconductor superlattices into semiconductor hyperbolic metamaterials (SHMs). In this paper, we investigate the optical properties associated with such ultrafast topological transitions. We first show reflectance, transmittance, and absorption under TE and TM plane wave incidence. In the unpumped state, the superlattice exhibits a frequency region with high reflectance (>80%) and a region with low reflectance (<1%) for both TE and TM polarizations over a wide range of incidence angles. In contrast, in the photopumped state, the reflectance for both frequencies and polarizations is very low (<1%) for a similar range of angles. Interestingly, this system can function as an all-optical reflection switch on ultrafast timescales. Furthermore, for TM incidence and close to the epsilon-near-zero point of the longitudinal permittivity, directional perfect absorption on ultrafast timescales may also be achieved. Finally, we discuss the onset of negative refraction in the photopumped state.
We have demonstrated single-mode lasing in a single gallium nitride nanowire using distributed feedback by external coupling to a dielectric grating. By adjusting the nanowire grating alignment we achieved a mode suppression ratio of 17dB.