Ligand Engineering and Recrystallization of Perovskite Quantum-Dot Thin Film for Low-Threshold Plasmonic Lattice Laser.

Solution-process perovskite quantum dots (QDs) are promising materials to be utilized in photovoltaics and photonics with their superior optical properties. Advancements in top-down nanofabrication for perovskite are thus important for practical photonic and plasmonic devices. However, different from the chemically synthesized nano/micro-structures that show high quality and low surface roughness, the perovskite QD thin film prepared by spin-coating or the drop-casting process shows a large roughness and inhomogeneity. Low-roughness and low-optical loss perovskite QD thin film is highly desired for photonic and optoelectronic devices. Here, this work presents a pressure-assisted ligand engineering/recrystallization process for high-quality and well-thickness controlled CsPbBr3 QD film and demonstrates a low-threshold and single-mode plasmonic lattice laser. A recrystallization process is proposed to prepare the QD film with a low roughness (RMS = 1.3 nm) and small thickness (100 nm). Due to the low scattering loss and strong interaction between gain media and plasmonic nanoparticles, a low lasing threshold of 16.9 µJ cm-2 is achieved. It is believed that this work is not only important to the plasmonic laser field but also provides a promising and general nanofabrication method of solution-processed QDs for various photonic and plasmonic devices.

Molecular dynamics study of water confined in MIL-101 metal-organic frameworks.

Molecular dynamics simulations of water adsorbed in Material Institute Lavoisier MIL-101(Cr) metal-organic frameworks are performed to analyze the kinetic properties of water molecules confined in the framework at 298.15 K and under different vapor pressures and clarify the water adsorption mechanism in MIL-101(Cr). The terahertz frequency-domain spectra (THz-FDS) of water are calculated by applying fast Fourier transform to the configurational data of water molecules. According to the characteristic frequencies in the THz-FDS, the dominant motions of water molecules in MIL-101(Cr) can be categorized into three types: (1) low-frequency translational motion (0-0.5 THz), (2) medium-frequency vibrational motion (2-2.5 THz), and (3) high-frequency vibrational motion (>6 THz). Each type of water motion is confirmed by visualizing the water configuration in MIL-101(Cr). The ratio of the number of water molecules with low-frequency translational motion to the total number of water molecules increases with the increase in vapor pressure. In contrast, that with medium-frequency vibrational motion is found to decrease with vapor pressure, exhibiting a pronounced decrease after water condensation has started in the cavities. That with the high-frequency vibrational motion is almost independent of the vapor pressure. The interactions between different types of water molecules affect the THz-FDS. Furthermore, the self-diffusion coefficient and the velocity auto-correlation function are calculated to clarify the adsorption state of the water confined in MIL-101(Cr). To confirm that the general trend of the THz-FDS does not depend on the water model, the simulations are performed using three water models, namely, rigid SPC/E, flexible SPC/E, and rigid TIP5PEw.

Engineering graphene and TMDs based van der Waals heterostructures for photovoltaic and photoelectrochemical solar energy conversion.

Graphene and two-dimensional (2D) transition metal dichalcogenides (TMDs) have attracted significant interest due to their unique properties that cannot be obtained in their bulk counterparts. These atomically thin 2D materials have demonstrated strong light-matter interactions, tunable optical bandgap structures and unique structural and electrical properties, rendering possible the high conversion efficiency of solar energy with a minimal amount of active absorber material. The isolated 2D monolayer can be stacked into arbitrary van der Waals (vdWs) heterostructures without the need to consider lattice matching. Several combinations of 2D/3D and 2D/2D materials have been assembled to create vdWs heterojunctions for photovoltaic (PV) and photoelectrochemical (PEC) energy conversion. However, the complex, less-constrained, and more environmentally vulnerable interface in a vdWs heterojunction is different from that of a conventional, epitaxially grown heterojunction, engendering new challenges for surface and interface engineering. In this review, the physics of band alignment, the chemistry of surface modification and the behavior of photoexcited charge transfer at the interface during PV and PEC processes will be discussed. We will present a survey of the recent progress and challenges of 2D/3D and 2D/2D vdWs heterojunctions, with emphasis on their applicability to PV and PEC devices. Finally, we will discuss emerging issues yet to be explored for 2D materials to achieve high solar energy conversion efficiency and possible strategies to improve their performance.

Combination of an Axicon Fiber Tip and a Camera Device into a Sensitive Refractive Index Sensor.

An axicon fiber tip combined with a camera device is developed to sensitively detect refractive indexes in solutions. The transparent axicon tips were made by etching optical fibers through a wet end-etching method at room temperature. When the axicon fiber tip was immersed in various refractive index media, the angular spectrum of the emitted light from the axicon fiber tip was changed. Using a low numerical aperture lens to collect the directly transmitted light, a high intensity sensitivity was achieved when the tip cone angle was about 35 to 40 degrees. We combined the axicon fiber tip with a laser diode and a smartphone into a portable refractometer. The front camera of the smartphone was used to collect the light emitted from the axicon fiber tip. By analyzing the selected area of the captured images, the refractive index can be distinguished for various solutions. The refractive index sensitivity was up to 56,000%/RIU, and the detection limit was 1.79 × 10-5 RIU. By measuring the refractive index change via the axicon fiber tip, the concentration of different mediums can be sensitively detected. The detection limits of the measurement for sucrose solutions, saline solutions, and diluted wine were 8.86 × 10-3 °Bx, 0.12‱, and 0.35%, respectively.

On-Chip Monolithically Fabricated Plasmonic-Waveguide Nanolaser.

Plasmonic-waveguide lasers, which exhibit subdiffraction limit lasing and light propagation, are promising for the next-generation of nanophotonic devices in computation, communication, and biosensing. Plasmonic lasers supporting waveguide modes are often based on nanowires grown with bottom-up techniques that need to be transferred and aligned for use in optical circuits. Here, we demonstrate a monolithically fabricated ZnO/Al plasmonic-waveguide nanolaser compatible with the fabrication requirements of on-chip circuits. The nanolaser is designed with a plasmonic metal layer on the top of the laser cavity only, providing highly efficient energy transfer between photons, excitons, and plasmons, and achieving lasing in the ultraviolet region up to 330 K with a low threshold intensity (0.20 mJ/cm2 at room temperature). This work demonstrates the realization of a plasmonic-waveguide nanolaser without the need for transfer and positioning steps, which is the key for on-chip integration of nanophotonic devices.

Plasmonic tooth-multilayer structure with high enhancement field for surface enhanced Raman spectroscopy.

The significant enhancement seen in surface-enhanced Raman scattering (SERS) heavily relies on the ability of plasmonic structures to strongly confine light. Current techniques used to fabricate plasmonic nanostructures have been limited in their reproducibility for bottom-up techniques or their feature size for top-down techniques. Here, we propose a tooth multilayer structure that can be fabricated by using physical vapor deposition and selective wet etching, achieving extremely small feature sizes and high reproducibility. A multilayer structure composed of two alternating materials whose thicknesses can be controlled accurately in the nanometer range is deposited on a flat substrate using ion-beam sputtering. Subsequent selective wet etching is used to form nanogaps in one of the materials constituting the multilayer, with the depth of the nanogaps being controlled by the wet etching time. Combining both techniques can allow the nanogap dimensions to be controlled at sub 10 nm length scale, thus achieving a tooth multilayer structure with high enhancement and tunability of the resonance mode over a broad range, ideal for SERS applications.

Spectrally Selective Photocapacitance Modulation in Plasmonic Nanochannels for Infrared Imaging.

The optical response of subwavelength plasmonic structures can be used to monitor minute changes in their physical, chemical, and biological environments with high performance for sensing. The optical response in the far field is governed by the near-field properties of plasmon resonances. Sharp, tunable resonances can be obtained by controlling the shape of the structure and by using resonant cavities. However, microintegration of plasmonic structures on chips is difficult because of the readout in the far field. As such, structures that form an electrical microcircuit and directly monitor the near-field variation would be more desirable. Here, we report on an electronically readable photocapacitor based on a plasmonic nanochannel structure with high spectral resolution and a large modulation capability. The structure consists of metallic U-cavities and semiconductor channels, which are used to focus and confine light at the semiconductor-metal interfaces. At these interfaces, light is efficiently converted into photocarriers that change the electrical impedance of the structure. The capacitance modulation of the structure in response to light produces a light-to-dark contrast ratio larger than 10(3). A reflectance spectrum with a bandwidth of 16 nm and a 6% modulation depth is detected using a reactance variation of 3 kΩ with the same bandwidth. This photocapacitor design offers a practical means of monitoring changes induced by the near field and thus could be deployed in pixel arrays of image sensors for miniaturized spectroscopic applications.

Fluid-controlled tunable infrared filtering in hollow plasmonic nanofin cavities.

Subwavelength structures sustaining surface plasmons have been employed in numerous fields due to their small size and ability to manipulate light beyond the diffraction limit. Light filtering using small-size plasmonic devices is a promising means of portable spectroscopy for purposes such as on-site chemical analyses. However, most plasmonic filters can only tune the resonance band by modifying the geometry of the structure or changing the incident light angle. Here, we present a plasmonic nanofin-cavity structure having a narrow band with its resonance wavelength controlled by varying the fluid in the hollow cavities of the filter. Control of the narrow-band resonance is realized over a wide range because of the coupling between the stationary surface plasmons generated from the nanofin-cavity mode and the propagating surface plasmons. The hollow cavity design enables fluid to be easily injected and removed, so that the filtered band can be controlled without the need for a complex and bulky structure or application of an external voltage.

Nanoporous CuO layer modified Cu electrode for high performance enzymatic and non-enzymatic glucose sensing.

Nanoporous CuO layer on Cu foil with a thick Cu2O interlayer is synthesized via post annealing of previously fabricated Cu(OH)2 nanowires at 500 °C under an oxygen flow. The formation of the thick sandwiched Cu2O layer is realized through the outward diffusion of Cu ions and subsequent oxidation. An O2 pressure above the dissociation pressure of CuO is used to form a CuO layer at the outer surface of the structure, thus realizing a low cost structure having a porous and high isoelectric point layer. The Cu/Cu2O/CuO structure is used as an efficient electrode for glucose sensing. Sensitivities of [Formula: see text] at 0.8 V versus Ag/AgCl and 1066 µA mM(-1) cm(-2) at 0.6 V versus Ag/AgCl are achieved in an enzymatic and non-enzymatic glucose sensing schemes, respectively. The improved electrochemical sensing ability might be attributed to the efficient electrocatalytic reaction on the high crystal quality CuO layer and the porous structure.

CuO nanowire/microflower/nanowire modified Cu electrode with enhanced electrochemical performance for non-enzymatic glucose sensing.

CuO nanowire/microflower structure on Cu foil is synthesized by annealing a Cu(OH)2 nanowire/CuO microflower structure at 250 °C in air. The nanowire/microflower structure with its large surface area leads to an efficient catalysis and charge transfer in glucose detection, achieving a high sensitivity of 1943 µA mM(-1) cm(-2), a wide linear range up to 4 mM and a low detection limit of 4 µM for amperometric glucose sensing in alkaline solution. With a second consecutive growth of CuO nanowires on the microflowers, the sensitivity of the obtained CuO nanowire/microflower/nanowire structure further increases to 2424 µA mM(-1) cm(-2), benefiting from an increased number of electrochemically active sites. The enhanced electrocatalytic performance of the CuO nanowire/microflower/nanowire electrode compared to the CuO nanowire/microflower electrode, CuO nanowire electrode and CuxO film electrode provides evidence for the significant role of available surface area for electrocatalysis. The rational combination of CuO nanowire and microflower nanostructures into a nanowire supporting microflower branching nanowires structure makes it a promising composite nanostructure for use in CuO based electrochemical sensors with promising analytical properties.

Fabrication of highly ordered Ta2O5 and Ta3N5 nanorod arrays by nanoimprinting and through-mask anodization.

Using highly ordered porous anodic alumina membrane fabricated with the aid of nanoimprinting as a mask, Ta2O5 nanorod array with uniform diameter, length, and distribution is grown in situ on a Ta substrate by through-mask anodization. The Ta2O5 nanorod array is further transformed into Ta3N5 nanorod array without damaging the nanorod structure by nitridation. Solar-driven photoelectrochemical water splitting with a maximum solar energy conversion efficiency of 0.36% is demonstrated with the Ta3N5 nanorod array after modifying the surface with cobalt-phosphate as a co-catalyst. The Ta2O5 and Ta3N5 nanorod arrays have potential applications in catalysis, photonics, UV photodetection and solar energy conversion.

Coupling of localized surface plasmons to U-shaped cavities for high-sensitivity and miniaturized detectors.

We report numerical analysis of the coupling of localized surface plasmons to the modes of U-shaped cavities. The coupling results in intense resonance for which the electric field is strongly enhanced on the cavity surfaces. As a result, an optical vortex in the power flow is formed in the cavities and a sharp and strong resonance dip is observed in the reflectance spectrum. High sensitivity of the dip wavelength to change in the refractive index of the surrounding medium is reported. The high sensitivity is realized with a small number of cavities, thus enabling miniaturization of detectors based on U-shaped cavities.

Plasmon focusing in short gold sphere nanochains for surface-enhanced Raman scattering.

Power-flow focusing in metal nanostructures is attracting growing attention to design efficient and tunable substrates for surface-enhanced Raman spectroscopy (SERS), and to propose a more reliable alternative to random surfaces for single-molecule sensing. In this paper, finite-difference time-domain simulations were used to explore the near-field amplification features of short chains of gold (Au) nanospheres. Short chains of gold spheres were found to induce stronger field enhancements than infinite chains due to a more efficient trapping and focusing of the incident energy. In addition, interaction with a suitably tuned SiO2/Au double-layer substrate was demonstrated to widen the resonance's bandwidth, meeting another practical need for SERS.

Angular Control of Circularly Polarized Emission from Achiral Molecules via Magnetic Dipoles Sustained in a Chiral Metamirror.

Circularly polarized emission (CPE) plays an important role in the designs of advanced displays and photonic integrated circuits. Unfortunately, the control of CPE handedness is limited by the chiral metasurfaces employed to emit chiral light. Particularly, the switching of the handedness with chiral metasurfaces relies on flipping the metasurfaces, which adds some constraints to practical applications. Herein, we propose an angle-sensitive chiral metamirror with Mie resonators to realize handedness switching. The Mie resonator supports a magnetic dipole having large field enhancement. This chiral metamirror is applied to excite CPEs with opposite handedness at emission angles within 10°. In contrast to the conventional methods, this work proposes a more efficient approach to manipulate the handedness of CPE.

High-Q lasing via all-dielectric Bloch-surface-wave platform.

Controlling the propagation and emission of light via Bloch surface waves (BSWs) has held promise in the field of on-chip nanophotonics. BSW-based optical devices are being widely investigated to develop on-chip integration systems. However, a coherent light source that is based on the stimulated emission of a BSW mode has yet to be developed. Here, we demonstrate lasers based on a guided BSW mode sustained by a gain-medium guiding structure microfabricated on the top of a BSW platform. A long-range propagation length of the BSW mode and a high-quality lasing emission of the BSW mode are achieved. The BSW lasers possess a lasing threshold of 6.7 µJ/mm2 and a very narrow linewidth reaching a full width at half maximum as small as 0.019 nm. Moreover, the proposed lasing scheme exhibits high sensitivity to environmental changes suggesting the applicability of the proposed BSW lasers in ultra-sensitive devices.

Chiroptical Response Inversion and Enhancement of Room-Temperature Exciton-Polaritons Using 2D Chirality in Perovskites.

Although chiral semiconductors have shown promising progress in direct circularly polarized light (CPL) detection and emission, they still face potential challenges. A chirality-switching mechanism or approach integrating two enantiomers is needed to discriminate the handedness of a given CPL; additionally, a large material volume is required for sufficient chiroptical interaction. These two requirements pose significant obstacles to the simplification and miniaturization of the devices. Here, room-temperature chiral polaritons fulfilling dual-handedness functions and exhibiting a more-than-two-order enhancement of the chiroptical signal are demonstrated, by embedding a 40 nm-thick perovskite film with a 2D chiroptical effect into a Fabry-Pérot cavity. By mixing chiral perovskites with different crystal structures, a pronounced 2D chiroptical effect is accomplished in the perovskite film, featured by an inverted chiroptical response for counter-propagating CPL. This inversion behavior matches the photonic handedness switch during CPL circulation in the Fabry-Pérot cavity, thus harvesting giant enhancement of the chiroptical response. Furthermore, affected by the unique quarter-wave-plate effects, the polariton emission achieves a chiral dissymmetry of ±4% (for the emission from the front and the back sides). The room-temperature polaritons with the strong dissymmetric chiroptical interaction shall have implications on a fundamental level and future on-chip applications for biomolecule analysis and quantum computing.

Sensitivity to refractive index of high-aspect-ratio nanofins with optical vortex.

An easy and large-scale fabrication technique of metal fins was used to produce periodic Au fin arrays that realized light confinement in the near-infrared region. Light confinement was revealed by vortex patterns in the optical power flow of an array of high-aspect-ratio fins (height of 1000 nm for a width of 50 nm). The light confinement resulted in sharp dips in the reflectance spectrum of the high-aspect-ratio fin array. The wavelengths of the reflectance dips were found to shift toward higher values when the refractive index of the surrounding medium was increased. Experimental and simulated dip shift values were in good agreement with a demonstrated sensitivity of 580 nm per refractive index unit.

ZnO dense nanowire array on a film structure in a single crystal domain texture for optical and photoelectrochemical applications.

A single crystal domain texture quality (a unique in-plane and out-of-plane crystalline orientation over a large area) ZnO nanostructure of a dense nanowire array on a thick film has been homogeneously synthesized on a-plane sapphire substrates over large areas through a one-step chemical vapor deposition (CVD) process. The growth mechanism is clarified: a single crystal [02(-)1] oriented ZnAl(2)O(4) buffer layer was formed at the ZnO film and the a-plane sapphire substrate interface via a diffusion reaction process during the CVD process, providing improved epitaxial conditions that enable the synthesis of the high crystalline quality ZnO nanowire array on a film structure. The high optoelectronic quality of the ZnO nanowire array on a film sample is evidenced by the free exitonic emissions in the low-temperature photoluminescence spectroscopy. A carrier density of ~10(17) cm(-3) with an n-type conductivity of the ZnO nanowire array on a film sample is obtained by electrochemical impedance analysis. Finally, the ZnO nanowire array on a film sample is demonstrated to be an ideal template for a further synthesis of a single crystal quality ZnO-ZnGa(2)O(4) core-shell nanowire array on a film structure. The fabricated ZnO-ZnGa(2)O(4) sample revealed an enhanced anticorrosive ability and photoelectrochemical performance when used as a photoanode in a photoelectrochemical water splitting application.

Near-Zero-Index Slabs on Bloch Surface Wave Platform for Long-Range Directional Couplers and Optical Logic Gates.

Near-zero-index materials and structures, with their extraordinary optical behaviors of phase-free propagation resulting in directional radiation, provide a possible approach for directional coupling and optical logic gates in photonic integrated circuits. However, the radiation from the near-zero-index structures is limited to a short range of a few hundreds of nanometers. A Bloch surface wave (BSW), an electromagnetic surface wave that can be excited at the interface between an all-dielectric multilayer and a dielectric medium with a low-loss optical mode, provides a solution to increase the propagation length. In this work, we present a nanostructured near-zero-index slab integrated on the all-dielectric metal-free BSW platform for long-range surface wave radiation. By employing the long-range directional surface-wave radiation, a directional coupler and optical logic gates based on the BSW near-zero-index slabs are realized. The proposed directional couplers achieve long coupling distances (the electric-field magnitude ratio between the input slab and output slab is 0.22 with a 50 µm coupling distance), which is 2 orders of magnitude longer than that of conventional directional couplers based on evanescent wave coupling. By controlling the interference pattern of the BSW between the slabs, the XOR logic gate is experimentally demonstrated with a significant extinction ratio of 27.9 dB at telecommunications wavelengths. The BSW near-zero-index logic gates and the directional coupler with long-range light propagation provide an approach to the development of photonic integrated circuits and metal-free surface wave-based applications.

Integration of on-chip perovskite nanocrystal laser and long-range surface plasmon polariton waveguide with etching-free process.

Perovskite materials prepared in the form of solution-processed nanocrystals and used in top-down fabrication techniques are very attractive to develop low-cost and high-quality integrated optoelectronic circuits. Particularly, integrated miniaturized coherent light sources that can be connected to light-guiding structures on a chip are highly desired. To control light propagating on a small footprint with low-loss optical modes, long-range surface plasmon polariton (LRSPP) waveguides are employed. Herein, we demonstrate an on-chip fabricated photonic-plasmonic hybrid system consisting of a perovskite lasing structure coupled to an LRSPP waveguide achieving a low lasing threshold and a propagation length over 100 µm. Preventing perovskite material degradation and the formation of surface roughness of the laser cavity during fabrication is made possible by designing a fabrication technique without any etching step.