Temperature-Dependent Excitonic Light Manipulation with Atomically Thin Optical Elements.

Monolayer 2D semiconductors, such as WS2, exhibit uniquely strong light-matter interactions due to exciton resonances that enable atomically thin optical elements. Similar to geometry-dependent plasmon and Mie resonances, these intrinsic material resonances offer coherent and tunable light scattering. Thus far, the impact of the excitons' temporal dynamics on the performance of such excitonic metasurfaces remains unexplored. Here, we show how the excitonic decay rates dictate the focusing efficiency of an atomically thin lens carved directly out of exfoliated monolayer WS2. By isolating the coherent exciton radiation from the incoherent background in the focus of the lens, we obtain a direct measure of the role of exciton radiation in wavefront shaping. Furthermore, we investigate the influence of exciton-phonon scattering by characterizing the focusing efficiency as a function of temperature, demonstrating an increased optical efficiency at cryogenic temperatures. Our results provide valuable insights into the role of excitonic light scattering in 2D nanophotonic devices.

Spectrally interleaved topologies using geometric phase metasurfaces.

Metasurfaces facilitate the interleaving of multiple topologies in an ultra-thin photonic system. Here, we report on the spectral interleaving of topological states of light using a geometric phase metasurface. We realize that a dielectric spectrally interleaved metasurface generates multiple interleaved vortex beams at different wavelengths. By harnessing the space-variant polarization manipulations that are enabled by the geometric phase mechanism, a vectorial vortex array is implemented. The presented interleaved topologies concept can greatly enhance the functionality of advanced microscopy and communication systems.

Switching of Photonic Crystal Lasers by Graphene.

Unique features of graphene have motivated the development of graphene-integrated photonic devices. In particular, the electrical tunability of graphene loss enables high-speed modulation of light and tuning of cavity resonances in graphene-integrated waveguides and cavities. However, efficient control of light emission such as lasing, using graphene, remains a challenge. In this work, we demonstrate on/off switching of single- and double-cavity photonic crystal lasers by electrical gating of a monolayer graphene sheet on top of photonic crystal cavities. The optical loss of graphene was controlled by varying the gate voltage Vg, with the ion gel atop the graphene sheet. First, the fundamental properties of graphene were investigated through the transmittance measurement and numerical simulations. Next, optically pumped lasing was demonstrated for a graphene-integrated single photonic crystal cavity at Vg below -0.6 V, exhibiting a low lasing threshold of ∼480 µW, whereas lasing was not observed at Vg above -0.6 V owing to the intrinsic optical loss of graphene. Changing quality factor of the graphene-integrated photonic crystal cavity enables or disables the lasing operation. Moreover, in the double-cavity photonic crystal lasers with graphene, switching of individual cavities with separate graphene sheets was achieved, and these two lasing actions were controlled independently despite the close distance of ∼2.2 µm between adjacent cavities. We believe that our simple and practical approach for switching in graphene-integrated active photonic devices will pave the way toward designing high-contrast and ultracompact photonic integrated circuits.

High Resolution Full-Aperture ISAR Processing through Modified Doppler History Based Motion Compensation.

A high resolution inverse synthetic aperture radar (ISAR) technique is presented using modified Doppler history based motion compensation. To this purpose, a novel wideband ISAR system is developed that accommodates parametric processing over extended aperture length. The proposed method is derived from an ISAR-to-SAR approach that makes use of high resolution spotlight SAR and sub-aperture recombination. It is dedicated to wide aperture ISAR imaging and exhibits robust performance against unstable targets having non-linear motions. We demonstrate that the Doppler histories of the full aperture ISAR echoes from disturbed targets are efficiently retrieved with good fitting models. Experiments have been conducted on real aircraft targets and the feasibility of the full aperture ISAR processing is verified through the acquisition of high resolution ISAR imagery.

Microstructured Air Cavities as High-Index Contrast Substrates with Strong Diffraction for Light-Emitting Diodes.

Two-dimensional high-index-contrast dielectric gratings exhibit unconventional transmission and reflection due to their morphologies. For light-emitting devices, these characteristics help guided modes defeat total internal reflections, thereby enhancing the outcoupling efficiency into an ambient medium. However, the outcoupling ability is typically impeded by the limited index contrast given by pattern media. Here, we report strong-diffraction, high-index-contrast cavity engineered substrates (CESs) in which hexagonally arranged hemispherical air cavities are covered with a 80 nm thick crystallized alumina shell. Wavelength-resolved diffraction measurements and Fourier analysis on GaN-grown CESs reveal that the high-index-contrast air/alumina core/shell patterns lead to dramatic excitation of the low-order diffraction modes. Large-area (1075 × 750 µm(2)) blue-emitting InGaN/GaN light-emitting diodes (LEDs) fabricated on a 3 µm pitch CES exhibit ∼39% enhancement in the optical power compared to state-of-the-art, patterned-sapphire-substrate LEDs, while preserving all of the electrical metrics that are relevant to LED devices. Full-vectorial simulations quantitatively demonstrate the enhanced optical power of CES LEDs and show a progressive increase in the extraction efficiency as the air cavity volume is expanded. This trend in light extraction is observed for both lateral- and flip-chip-geometry LEDs. Measurements of far-field profiles indicate a substantial beaming effect for CES LEDs, despite their few-micron-pitch pattern. Near-to-far-field transformation simulations and polarization analysis demonstrate that the improved extraction efficiency of CES LEDs is ascribed to the increase in emissions via the top escape route and to the extraction of transverse-magnetic polarized light.

Resonant magneto-optic Kerr effects of a single Ni nanorod in the Mie scattering regime.

We present a systematic, theoretical investigation of the polar magneto-optical (MO) Kerr effects of a single Ni nanorod in the Mie regime. The MO Kerr rotation, ellipticity, amplitude ratio, and phase shift are calculated as a function of the length and width of the nanorod. The electric field amplitude ratio of the MO Kerr effect is locally maximized when the nanorod supports a plasmonic resonance in the polarization state orthogonal to the incident light. The plasmonic resonances directly induced by the incident light do not enhance the amplitude ratio. In the Mie regime, multiple local maxima of the MO Kerr activity are supported by the resonant modes with different modal characteristics. From the viewpoint of first-order perturbation analysis, the spatial overlap between the incident-light-induced electric field and the Green function determines the local maxima.

Full three-dimensional power flow analysis of single-emitter-plasmonic-nanoantenna system.

We present a full three-dimensional (3D) power flow analysis of an emitter-nanoantenna system. A conventional analysis, based on the total Poynting vector, calculates only the coupling strength in terms of the Purcell enhancement. For a better understanding of the emitter-nanoantenna system, not only the Purcell enhancement but also complete information on the energy transfer channels is necessary. The separation of the pure scattering and emitter output Poynting vectors enables the quantification of the individual energy transfer channels. Employing the finite-difference time-domain method (FDTD), we examine a nanodisk antenna that supports the bright dipole and dark quadrupole resonance modes for which the power flow characteristics are completely distinct, and we analyze the power flow enhancements to the energy transfer channels with respect to the wavelength, polarization, and position of the emitter coupled to the antenna. The 3D power flow analysis reveals how the constructive or destructive interference between the emitter and the antenna resonance mode affects the power flow enhancements and the far-field radiation pattern. Our proposed power flow analysis should play a critical role in characterizing the emitter-antenna system and customizing its energy transfer properties for desired applications.

Plasmonic nano-comb structures for efficient large-area second harmonic generation.

We propose and demonstrate plasmonic nano-comb (PNC) structures for efficient large-area second-harmonic generation (SHG). The PNCs are made of 250 nm-thick gold film and have equally-spaced 30 nm-slits filled with ployvinylidene fluoride-co-trifluoroethylene (P(VDF-TrFE)). The PNC with 1.0 µm-spacing couples resonantly with 1.56 µm 100-fs laser beams. For the 1.0 µm-spacing PNCs under the fixed-pump-power condition, the nonlinear SHG power remains almost independent of the pump diameter ranging from 2 µm to 6 µm. The SHG power from the resonant PNC is measured to be 8 times larger than that of the single-nano-gap metallic structure, when the pump beam is tightly-focused to 2 µm in diameter in both cases. This relative enhancement of the total nonlinear SHG signal power reaches up to >200 when the pump beam diameter is increased to 6 µm. We attribute this unusual phenomenon to the resonant coupling of the finite-size pump wave with the finite-size one-dimensional plasmonic mode.

Design of plasmonic nano-antenna for total internal reflection fluorescence microscopy.

We propose a gold modified bow-tie plasmonic nano-antenna, which can be suitably used in combination with total internal reflection fluorescence microscopy. The plasmonic nano-antenna, supporting well-separated multiple resonances, not only concentrates the total internal reflection evanescent field at the deep subwavelength scale, but also enhances fluorescence emission by the Purcell effect. Finite-difference time-domain computations show that the enhancement of the excitation light strongly correlates with the far-field radiation pattern radiated from the antenna. Depending on the antenna geometry, the resonant modes are widely tuned and their wavelengths can be easily matched to the diverse emission or excitation wavelengths of fluorophores.

Semiconducting [(Bi4Te4Br2)(Al2Cl(6-x)Br(x))]Cl2 and [Bi2Se2Br](AlCl4): cationic chalcogenide frameworks from Lewis acidic ionic liquids.

Lewis acidic organic ionic liquids provide a novel synthetic medium to prepare new semiconducting chalcogenides, [(Bi4Te4Br2)(Al2Cl5.46Br0.54)]Cl2 (1) and [Bi2Se2Br](AlCl4) (2). Compound 1 features a cationic [(Bi4Te4Br2)(Al2Cl5.46Br0.54)](2+) three-dimensional framework, while compound 2 consists of cationic layers of [Bi2Se2Br](2+). Spectroscopically measured band gaps of 1 and 2 are ∼0.6 and ∼1.2 eV, respectively. Thermoelectric power measurements of single crystals of 1 indicate an n-type semiconductor.

Off-axis metasurfaces for folded flat optics.

The overall size of an optical system is limited by the volume of the components and the internal optical path length. To reach the limits of miniaturization, it is possible to reduce both component volume and path length by combining the concepts of metasurface flat optics and folded optics. In addition to their subwavelength component thickness, metasurfaces enable bending conventional folded geometries off axis beyond the law of reflection. However, designing metasurfaces for highly off-axis illumination with visible light in combination with a high numerical aperture is non-trivial. In this case, traditional designs with gradient metasurfaces exhibit low diffraction efficiencies and require the use of deep-subwavelength, high-index, and high-aspect-ratio semiconductor nanostructures that preclude inexpensive, large-area nanofabrication. Here, we describe a design approach that enables the use of low-index (n ≈ 1.5), low-aspect ratio structures for off-axis metagratings that can redirect and focus visible light (λ = 532 nm) with near-unity efficiency. We show that fabricated optical elements offer a very large angle-of-view (110°) and lend themselves to scalable fabrication by nano-imprint lithography.

CsSnI3: Semiconductor or metal? High electrical conductivity and strong near-infrared photoluminescence from a single material. High hole mobility and phase-transitions.

CsSnI(3) is an unusual perovskite that undergoes complex displacive and reconstructive phase transitions and exhibits near-infrared emission at room temperature. Experimental and theoretical studies of CsSnI(3) have been limited by the lack of detailed crystal structure characterization and chemical instability. Here we describe the synthesis of pure polymorphic crystals, the preparation of large crack-/bubble-free ingots, the refined single-crystal structures, and temperature-dependent charge transport and optical properties of CsSnI(3), coupled with ab initio first-principles density functional theory (DFT) calculations. In situ temperature-dependent single-crystal and synchrotron powder X-ray diffraction studies reveal the origin of polymorphous phase transitions of CsSnI(3). The black orthorhombic form of CsSnI(3) demonstrates one of the largest volumetric thermal expansion coefficients for inorganic solids. Electrical conductivity, Hall effect, and thermopower measurements on it show p-type metallic behavior with low carrier density, despite the optical band gap of 1.3 eV. Hall effect measurements of the black orthorhombic perovskite phase of CsSnI(3) indicate that it is a p-type direct band gap semiconductor with carrier concentration at room temperature of ∼ 10(17) cm(-3) and a hole mobility of ∼585 cm(2) V(-1) s(-1). The hole mobility is one of the highest observed among p-type semiconductors with comparable band gaps. Its powders exhibit a strong room-temperature near-IR emission spectrum at 950 nm. Remarkably, the values of the electrical conductivity and photoluminescence intensity increase with heat treatment. The DFT calculations show that the screened-exchange local density approximation-derived band gap agrees well with the experimentally measured band gap. Calculations of the formation energy of defects strongly suggest that the electrical and light emission properties possibly result from Sn defects in the crystal structure, which arise intrinsically. Thus, although stoichiometric CsSnI(3) is a semiconductor, the material is prone to intrinsic defects associated with Sn vacancies. This creates highly mobile holes which cause the materials to appear metallic.

Metasurface optofluidics for dynamic control of light fields.

The ability to manipulate light and liquids on integrated optofluidics chips has spurred a myriad of important developments in biology, medicine, chemistry and display technologies. Here we show how the convergence of optofluidics and metasurface optics can lead to conceptually new platforms for the dynamic control of light fields. We first demonstrate metasurface building blocks that display an extreme sensitivity in their scattering properties to their dielectric environment. These blocks are then used to create metasurface-based flat optics inside microfluidic channels where liquids with different refractive indices can be directed to manipulate their optical behaviour. We demonstrate the intensity and spectral tuning of metasurface colour pixels as well as on-demand optical elements. We finally demonstrate automated control in an integrated meta-optofluidic platform to open up new display functions. Combined with large-scale microfluidic integration, our dynamic-metasurface flat-optics platform could open up the possibility of dynamic display, imaging, holography and sensing applications.

Quantitative phase contrast imaging with a nonlocal angle-selective metasurface.

Phase contrast microscopy has played a central role in the development of modern biology, geology, and nanotechnology. It can visualize the structure of translucent objects that remains hidden in regular optical microscopes. The optical layout of a phase contrast microscope is based on a 4 f image processing setup and has essentially remained unchanged since its invention by Zernike in the early 1930s. Here, we propose a conceptually new approach to phase contrast imaging that harnesses the non-local optical response of a guided-mode-resonator metasurface. We highlight its benefits and demonstrate the imaging of various phase objects, including biological cells, polymeric nanostructures, and transparent metasurfaces. Our results showcase that the addition of this non-local metasurface to a conventional microscope enables quantitative phase contrast imaging with a 0.02π phase accuracy. At a high level, this work adds to the growing body of research aimed at the use of metasurfaces for analog optical computing.

Thallium chalcohalides for X-ray and γ-ray detection.

We report that the chalcohalide compound Tl(6)SeI(4) is a promising material for efficient X-ray and γ-ray detection. This material has a higher figure of merit than the current state-of-the-art material for room-temperature operation, Cd(0.9)Zn(0.1)Te (CZT). We have synthesized high-quality single-crystalline wafers of Tl(6)SeI(4) with detector-grade resistivities and good carrier transport of both electrons and holes. We demonstrate that pulse height spectra recorded using Co-57 radiation show an energy resolution matching that of a commercial CZT detector material.

Optical recoil of asymmetric nano-optical antenna.

We propose nano-optical antennas with asymmetric radiation patterns as light-driven mechanical recoil force generators. Directional antennas are found to generate recoil force efficiently when driven in the spectral proximity of their resonances. It is also shown that the recoil force is equivalent to the Poynting vector integrated over a closed sphere containing the antenna structures.

Non-local metasurfaces for spectrally decoupled wavefront manipulation and eye tracking.

Metasurface-based optical elements typically manipulate light waves by imparting space-variant changes in the amplitude and phase with a dense array of scattering nanostructures. The highly localized and low optical-quality-factor (Q) modes of nanostructures are beneficial for wavefront shaping as they afford quasi-local control over the electromagnetic fields. However, many emerging imaging, sensing, communication, display and nonlinear optics applications instead require flat, high-Q optical elements that provide substantial energy storage and a much higher degree of spectral control over the wavefront. Here, we demonstrate high-Q, non-local metasurfaces with atomically thin metasurface elements that offer notably enhanced light-matter interaction and fully decoupled optical functions at different wavelengths. We illustrate a possible use of such a flat optic in eye tracking for eyewear. Here, a metasurface patterned on a regular pair of eye glasses provides an unperturbed view of the world across the visible spectrum and redirects near-infrared light to a camera to allow imaging of the eye.

Nanoelectromechanical modulation of a strongly-coupled plasmonic dimer.

The ability of two nearly-touching plasmonic nanoparticles to squeeze light into a nanometer gap has provided a myriad of fundamental insights into light-matter interaction. In this work, we construct a nanoelectromechanical system (NEMS) that capitalizes on the unique, singular behavior that arises at sub-nanometer particle-spacings to create an electro-optical modulator. Using in situ electron energy loss spectroscopy in a transmission electron microscope, we map the spectral and spatial changes in the plasmonic modes as they hybridize and evolve from a weak to a strong coupling regime. In the strongly-coupled regime, we observe a very large mechanical tunability (~250 meV/nm) of the bonding-dipole plasmon resonance of the dimer at ~1 nm gap spacing, right before detrimental quantum effects set in. We leverage our findings to realize a prototype NEMS light-intensity modulator operating at ~10 MHz and with a power consumption of only 4 fJ/bit.

Synthesis in ionic liquids: [Bi2Te2Br](AlCl4), a direct gap semiconductor with a cationic framework.

The Lewis acidic ionic liquid EMIMBr-AlCl(3) (EMIM = 1-ethyl-3-methylimidazolium) allows a novel synthetic route to the semiconducting layered metal chalcogenides halide [Bi(2)Te(2)Br](AlCl(4)) and its Sb analogue. [Bi(2)Te(2)Br](AlCl(4)) is a direct band gap, strongly anisotropic semiconductor and consists of cationic infinite layers of [Bi(2)Te(2)Br](+) and [AlCl(4)](-) anions inserted between the layers.

Soluble semiconductors AAsSe2 (A = Li, Na) with a direct-band-gap and strong second harmonic generation: a combined experimental and theoretical study.

AAsSe(2) (A = Li, Na) have been identified as a new class of polar direct-band gap semiconductors. These I-V-VI(2) ternary alkali-metal chalcoarsenates have infinite single chains of (1/infinity)[AsQ(2)(-)] derived from corner-sharing pyramidal AsQ(3) units with stereochemically active lone pairs of electrons on arsenic. The conformations and packing of the chains depend on the structure-directing alkali metals. This results in at least four different structural types for the Li(1-x)Na(x)AsSe(2) stoichiometry (alpha-LiAsSe(2), beta-LiAsSe(2), gamma-NaAsSe(2), and delta-NaAsSe(2)). Single-crystal X-ray diffraction studies showed an average cubic NaCl-type structure for alpha-LiAsSe(2), which was further demonstrated to be locally distorted by pair distribution function (PDF) analysis. The beta and gamma forms have polar structures built of different (1/infinity)[AsSe(2)(-)] chain conformations, whereas the delta form has nonpolar packing. A wide range of direct band gaps are observed, depending on composition: namely, 1.11 eV for alpha-LiAsSe(2), 1.60 eV for LiAsS(2), 1.75 eV for gamma-NaAsSe(2), 2.23 eV for NaAsS(2). The AAsQ(2) materials are soluble in common solvents such as methanol, which makes them promising candidates for solution processing. Band structure calculations performed with the highly precise screened-exchange sX-LDA FLAPW method confirm the direct-gap nature and agree well with experiment. The polar gamma-NaAsSe(2) shows very large nonlinear optical (NLO) second harmonic generation (SHG) response in the wavelength range of 600-950 nm. The theoretical studies confirm the experimental results and show that gamma-NaAsSe(2) has the highest static SHG coefficient known to date, 337.9 pm/V, among materials with band gaps larger than 1.0 eV.