Terahertz Pulse Generation with Binary Phase Control in Nonlinear InAs Metasurface.

The effect of terahertz (THz) pulse generation has revolutionized broadband coherent spectroscopy and imaging at THz frequencies. However, THz pulses typically lack spatial structure, whereas structured beams are becoming essential for advanced spectroscopy applications. Nonlinear optical metasurfaces with nanoscale THz emitters can provide a solution by defining the beam structure at the generation stage. We develop a nonlinear InAs metasurface consisting of nanoscale optical resonators for simultaneous generation and structuring of THz beams. We find that THz pulse generation in the resonators is governed by optical rectification. It is more efficient than in ZnTe crystals, and it allows us to control the pulse polarity and amplitude, offering a platform for realizing binary-phase THz metasurfaces. To illustrate this capability, we demonstrate an InAs metalens, which simultaneously generates and focuses THz pulses. The control of spatiotemporal structure using nanoscale emitters opens doors for THz beam engineering and advanced spectroscopy and imaging applications.

Correction to "Terahertz Pulse Generation from GaAs Metasurfaces".

[This corrects the article DOI: 10.1021/acsphotonics.1c01908.].

Terahertz Pulse Generation from GaAs Metasurfaces.

Ultrafast optical excitation of select materials gives rise to the generation of broadband terahertz (THz) pulses. This effect has enabled the field of THz time-domain spectroscopy and led to the discovery of many physical mechanisms behind THz generation. However, only a few materials possess the required properties to generate THz radiation efficiently. Optical metasurfaces can relax stringent material requirements by shifting the focus onto the engineering of local electromagnetic fields to boost THz generation. Here we demonstrate the generation of THz pulses in a 160 nm thick nanostructured GaAs metasurface. Despite the drastically reduced volume, the metasurface emits THz radiation with efficiency comparable to that of a thick GaAs crystal. We reveal that along with classical second-order volume nonlinearity, an additional mechanism contributes strongly to THz generation in the metasurface, which we attribute to surface nonlinearity. Our results lay the foundation for engineering of semiconductor metasurfaces for efficient and versatile THz radiation emitters.

Liquid-Metal-Based Nanophotonic Structures for High-Performance SEIRA Sensing.

Surface-enhanced infrared absorption (SEIRA) spectroscopy can provide label-free, nondestructive detection and identification of analytes with high sensitivity and specificity, and therefore has been widely used for various sensing applications. SEIRA sensors usually employ resonant nanophotonic structures, which can substantially enhance the electric field and hence light-matter interactions by orders of magnitude in certain nanoscale hot spots of the devices. However, as ever, smaller hot spots are employed to further enhance the field, the delivery of analytes into such hot spots becomes increasingly challenging. Here, high-performance nanophotonic SEIRA sensors based on nanopatch antennas with a liquid gallium ground plane are demonstrated, which not only lead to ultrahigh field confinement and enhancement, but also allow for convenient and efficient delivery of analytes into nanometric hot spots by employing a simple procedure suitable for point-of-care applications. The sensors exhibit superior sensitivity in the midinfrared spectral region. Around 10% molecular vibrational signals (i.e., the modulation of a sensor's reflection spectrum owing to the molecular vibrational modes of the analytes) near 2900 cm-1  are achieved from sensing monolayer 1-octadecanethiol. This cost-effective and reliable method for realizing liquid-metal-based nanophotonic structures provides a new strategy for developing high-performance sensors and other photonics applications in the infrared region.

The Creation of True Two-Dimensional Silicon Carbide.

This paper reports the successful synthesis of true two-dimensional silicon carbide using a top-down synthesis approach. Theoretical studies have predicted that 2D SiC has a stable planar structure and is a direct band gap semiconducting material. Experimentally, however, the growth of 2D SiC has challenged scientists for decades because bulk silicon carbide is not a van der Waals layered material. Adjacent atoms of SiC bond together via covalent sp3 hybridization, which is much stronger than van der Waals bonding in layered materials. Additionally, bulk SiC exists in more than 250 polytypes, further complicating the synthesis process, and making the selection of the SiC precursor polytype extremely important. This work demonstrates, for the first time, the successful isolation of 2D SiC from hexagonal SiC via a wet exfoliation method. Unlike many other 2D materials such as silicene that suffer from environmental instability, the created 2D SiC nanosheets are environmentally stable, and show no sign of degradation. 2D SiC also shows interesting Raman behavior, different from that of the bulk SiC. Our results suggest a strong correlation between the thickness of the nanosheets and the intensity of the longitudinal optical (LO) Raman mode. Furthermore, the created 2D SiC shows visible-light emission, indicating its potential applications for light-emitting devices and integrated microelectronics circuits. We anticipate that this work will cause disruptive impact across various technological fields, ranging from optoelectronics and spintronics to electronics and energy applications.

Highly efficient terahertz photoconductive metasurface detectors operating at microwatt-level gate powers.

Despite their wide use in terahertz (THz) research and technology, the application spectra of photoconductive antenna (PCA) THz detectors are severely limited due to the relatively high optical gating power requirement. This originates from poor conversion efficiency of optical gate beam photons to photocurrent in materials with sub-picosecond carrier lifetimes. Here we show that using an ultra-thin (160 nm), perfectly absorbing low-temperature grown GaAs metasurface as the photoconductive channel drastically improves the efficiency of THz PCA detectors. This is achieved through perfect absorption of the gate beam in a significantly reduced photoconductive volume, enabled by the metasurface. This Letter demonstrates that sensitive THz PCA detection is possible using optical gate powers as low as 5 µW-three orders of magnitude lower than gating powers used for conventional PCA detectors. We show that significantly higher optical gate powers are not necessary for optimal operation, as they do not improve the sensitivity to the THz field. This class of efficient PCA THz detectors opens doors for THz applications with low gate power requirements.

All-optical switching of an epsilon-near-zero plasmon resonance in indium tin oxide.

Nonlinear optical devices and their implementation into modern nanophotonic architectures are constrained by their usually moderate nonlinear response. Recently, epsilon-near-zero (ENZ) materials have been found to have a strong optical nonlinearity, which can be enhanced through the use of cavities or nano-structuring. Here, we study the pump dependent properties of the plasmon resonance in the ENZ region in a thin layer of indium tin oxide (ITO). Exciting this mode using the Kretschmann-Raether configuration, we study reflection switching properties of a 60 nm layer close to the resonant plasmon frequency. We demonstrate a thermal switching mechanism, which results in a shift in the plasmon resonance frequency of 20 THz for a TM pump intensity of 70 GW cm-2. For degenerate pump and probe frequencies, we highlight an additional two-beam coupling contribution, not previously isolated in ENZ nonlinear optics studies, which leads to an overall pump induced change in reflection from 1% to 45%.

An In-situ and Direct Confirmation of Super-Planckian Thermal Radiation Emitted From a Metallic Photonic-Crystal at Optical Wavelengths.

Planck's law predicts the distribution of radiation energy, color and intensity, emitted from a hot object at thermal equilibrium. The Law also sets the upper limit of radiation intensity, the blackbody limit. Recent experiments reveal that micro-structured tungsten can exhibit significant deviation from the blackbody spectrum. However, whether thermal radiation with weak non-equilibrium pumping can exceed the blackbody limit in the far field remains un-answered experimentally. Here, we compare thermal radiation from a micro-cavity/tungsten photonic crystal (W-PC) and a blackbody, which are both measured from the same sample and also in-situ. We show that thermal radiation can exceed the blackbody limit by >8 times at λ = 1.7 µm resonant wavelength in the far-field. Our observation is consistent with a recent calculation by Wang and John performed for a 2D W-PC filament. This finding is attributed to non-equilibrium excitation of localized surface plasmon resonances coupled to nonlinear oscillators and the propagation of the electromagnetic waves through non-linear Bloch waves of the W-PC structure. This discovery could help create super-intense narrow band thermal light sources and even an infrared emitter with a laser-like input-output characteristic.

Observation of Intersubband Polaritons in a Single Nanoantenna Using Nano-FTIR Spectroscopy.

Strong coupling of an intersubband (ISB) electron transition in quantum wells to a subwavelength plasmonic nanoantenna can give rise to intriguing quantum phenomena, such as ISB polariton condensation, and enable practical devices including low threshold lasers. However, experimental observation of ISB polaritons in an isolated subwavelength system has not yet been reported. Here, we use scanning probe near-field microscopy and Fourier-transform infrared (FTIR) spectroscopy to detect formation of ISB polariton states in a single nanoantenna. We excite the nanoantenna by a broadband IR pulse and spectrally analyze evanescent fields on the nanoantenna surface. We observe the distinctive splitting of the nanoantenna resonance peak into two polariton modes and two π-phase steps corresponding to each of the modes. We map ISB polariton dispersion using a set of nanoantennae of different sizes. This nano-FTIR spectroscopy approach opens doors for investigations of ISB polariton physics in the single subwavelength nanoantenna regime.

Terahertz Detection with Perfectly-Absorbing Photoconductive Metasurface.

Terahertz (THz) photoconductive devices are used for generation, detection, and modulation of THz waves, and they rely on the ability to switch electrical conductivity on a subpicosecond time scale using optical pulses. However, fast and efficient conductivity switching with high contrast has been a challenge, because the majority of photoexcited charge carriers in the switch do not contribute to the photocurrent due to fast recombination. Here, we improve efficiency of electrical conductivity switching using a network of electrically connected nanoscale GaAs resonators, which form a perfectly absorbing photoconductive metasurface. We achieve perfect absorption without incorporating metallic elements, by breaking the symmetry of cubic Mie resonators. As a result, the metasurface can be switched between conductive and resistive states with extremely high contrast using an unprecedentedly low level of optical excitation. We integrate this metasurface with a THz antenna to produce an efficient photoconductive THz detector. The perfectly absorbing photoconductive metasurface opens paths for developing a wide range of efficient optoelectronic devices, where required optical and electronic properties are achieved through nanostructuring the resonator network.

Single-shot on-chip spectral sensors based on photonic crystal slabs.

Miniaturized spectrometers have significant potential for portable applications such as consumer electronics, health care, and manufacturing. These applications demand low cost and high spectral resolution, and are best enabled by single-shot free-space-coupled spectrometers that also have sufficient spatial resolution. Here, we demonstrate an on-chip spectrometer that can satisfy all of these requirements. Our device uses arrays of photodetectors, each of which has a unique responsivity with rich spectral features. These responsivities are created by complex optical interference in photonic-crystal slabs positioned immediately on top of the photodetector pixels. The spectrometer is completely complementary metal-oxide-semiconductor (CMOS) compatible and can be mass produced at low cost.

Formation of self-assembled gold nanoparticle supercrystals with facet-dependent surface plasmonic coupling.

Metallic nanoparticles, such as gold and silver nanoparticles, can self-assemble into highly ordered arrays known as supercrystals for potential applications in areas such as optics, electronics, and sensor platforms. Here we report the formation of self-assembled 3D faceted gold nanoparticle supercrystals with controlled nanoparticle packing and unique facet-dependent optical property by using a binary solvent diffusion method. The nanoparticle packing structures from specific facets of the supercrystals are characterized by small/wide-angle X-ray scattering for detailed reconstruction of nanoparticle translation and shape orientation from mesometric to atomic levels within the supercrystals. We discover that the binary diffusion results in hexagonal close packed supercrystals whose size and quality are determined by initial nanoparticle concentration and diffusion speed. The supercrystal solids display unique facet-dependent surface plasmonic and surface-enhanced Raman characteristics. The ease of the growth of large supercrystal solids facilitates essential correlation between structure and property of nanoparticle solids for practical integrations.

Nonpolar InGaN/GaN Core-Shell Single Nanowire Lasers.

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.

Polarization control in GaN nanowire lasers.

We demonstrate polarization control in optically-pumped single GaN nanowire lasers fabricated by a top-down method. By placing the GaN nanowires onto gold substrates, the naturally occurring randomly orientated elliptical polarization of nanowire lasers is converted to a linear polarization that is oriented parallel to the substrate surface. Confirmed by simulation results, this polarization control is attributed to a polarization-dependent loss induced by the gold substrate, which breaks the mode degeneracy of the nanowire and forms two orthogonally polarized modes with largely different cavity losses.

Tailoring directional scattering through magnetic and electric resonances in subwavelength silicon nanodisks.

Interference of optically induced electric and magnetic modes in high-index all-dielectric nanoparticles offers unique opportunities for tailoring directional scattering and engineering the flow of light. In this article we demonstrate theoretically and experimentally that the interference of electric and magnetic optically induced modes in individual subwavelength silicon nanodisks can lead to the suppression of resonant backscattering and to enhanced resonant forward scattering of light. To this end we spectrally tune the nanodisk's fundamental electric and magnetic resonances with respect to each other by a variation of the nanodisk aspect ratio. This ability to tune two modes of different character within the same nanoparticle provides direct control over their interference, and, in consequence, allows for engineering the particle's resonant and off-resonant scattering patterns. Most importantly, measured and numerically calculated transmittance spectra reveal that backward scattering can be suppressed and forward scattering can be enhanced at resonance for the particular case of overlapping electric and magnetic resonances. Our experimental results are in good agreement with calculations based on the discrete dipole approach as well as finite-integral frequency-domain simulations. Furthermore, we show useful applications of silicon nanodisks with tailored resonances as optical nanoantennas with strong unidirectional emission from a dipole source.

Single-mode GaN nanowire lasers.

We demonstrate stable, single-frequency output from single, as-fabricated GaN nanowire lasers operating far above lasing threshold. Each laser is a linear, double-facet GaN nanowire functioning as gain medium and optical resonator, fabricated by a top-down technique that exploits a tunable dry etch plus anisotropic wet etch for precise control of the nanowire dimensions and high material gain. A single-mode linewidth of ~0.12 nm and >18 dB side-mode suppression ratio are measured. Numerical simulations indicate that single-mode lasing arises from strong mode competition and narrow gain bandwidth.

Nano-lithographically fabricated titanium dioxide based visible frequency three dimensional gap photonic crystal.

Photonic crystals (PC) have emerged as important types of structures for light manipulation. Ultimate control of light is possible by creating PCs with a complete three dimensional (3D) gap [1, 2]. This has proven to be a considerable challenge in the visible and ultraviolet frequencies mainly due to complications in integrating transparent, high refractive index (n) materials with fabrication techniques to create ~ 100nm features with long range translational order. In this letter, we demonstrate a nano-lithography approach based on a multilevel electron beam direct write and physical vapor deposition, to fabricate four-layer titania woodpile PCs that potentially exhibit complete 3D gap at visible wavelengths. We achieved a short wavelength bandedge of 525nm with a 300nm lattice constant PC. Due to the nanoscale precision and capability for defect control, the nanolithography approach represents an important step toward novel visible photonic devices for lighting, lasers, sensing and biophotonics.