Perovskite Light-Emitting Electrochemical Cells Employing Electron Injection/Transport Layers of Ionic Transition Metal Complexes.

Recently, perovskites have attracted intense attention due to their high potential in optoelectronic applications. Employing perovskites as the emissive materials of light-emitting electrochemical cells (LECs) shows the advantages of simple fabrication process, low-voltage operation, and compatibility with inert electrodes, along with saturated electroluminescence (EL) emission. Unlike in previously reported perovskite LECs, in which salts are incorporated in the emissive layer, the ion-transport layer was separated from the emissive layer in this work. The layer of ionic transition metal complex (iTMC) not only provides mobile ions but also serves as an electron-injection/transport layer. Orthogonal solvents are used in spin coating to prevent the intermixing of stacked perovskite and iTMC layers. The blue iTMC with high ionization potential is effective in blocking holes from the emissive layer and thus ensures EL color saturation. In addition, the carrier balance of the perovskite/iTMC LECs can be optimized by adjusting the iTMC layer thickness. The optimized external quantum efficiency of the CsPbBr3 /iTMC LEC reaches 6.8 %, which is among the highest reported values for perovskite LECs. This work successfully demonstrates that, compared with mixing all components in a single emissive layer, separating the layer of ion transport, electron injection and transport from the perovskite emissive layer is more effective in adjusting device carrier balance. As such, solution-processable perovskite/iTMC LECs open up a new way to realize efficient perovskite LECs.

Perovskite Light-Emitting Electrochemical Cells Employing Electron Injection/Transport Layers of Ionic Transition Metal Complexes.

Invited for the cover of this issue are Chin-Wei Lu, Zu-Po Yang, Hai-Ching Su, and co-workers at National Yang Ming Chiao Tung University and Providence University. The image depicts electron transport for light-emitting electrochemical cells. Read the full text of the article at 10.1002/chem.202103739.

Hybrid White-Light-Emitting Electrochemical Cells Based on a Blue Cationic Iridium(III) Complex and Red Quantum Dots.

Solid-state white light-emitting electrochemical cells (LECs) show promising advantages of simple solution fabrication processes, low operation voltage, and compatibility with air-stable cathode metals, which are required for lighting applications. To date, white LECs based on ionic transition metal complexes (iTMCs) have shown higher device efficiencies than white LECs employing other types of materials. However, lower emission efficiencies of red iTMCs limit further improvement in device performance. As an alternative, efficient red CdZnSeS/ZnS core/shell quantum dots were integrated with a blue iTMC to form a hybrid white LEC in this work. By achieving good carrier balance in an appropriate device architecture, a peak external quantum efficiency and power efficiency of 11.2 % and 15.1 lm W-1, respectively, were reached. Such device efficiency is indeed higher than those of the reported white LECs based on host-guest iTMCs. Time- and voltage-dependent electroluminescence (EL) characteristics of the hybrid white LECs were studied by means of the temporal evolution of the emission-zone position extracted by fitting the simulated and measured EL spectra. The working principle of the hybrid white LECs was clarified, and the high device efficiency makes potential new white-emitting devices suitable for solid-state lighting technology possible.

Cationic IrIII Emitters with Near-Infrared Emission Beyond 800†nm and Their Use in Light-Emitting Electrochemical Cells.

Solid-state near-infrared (NIR) light-emitting devices have recently received considerable attention as NIR light sources that can penetrate deep into human tissue and are suitable for bioimaging and labeling. In addition, solid-state NIR light-emitting electrochemical cells (LECs) have shown several promising advantages over NIR organic light-emitting devices (OLEDs). However, among the reported NIR LECs based on ionic transition-metal complexes (iTMCs), there is currently no iridium-based LEC that displays NIR electroluminescence (EL) peaks near to or above 800 nm. In this report we demonstrate a simple method for adjusting the energy gap between the highest-occupied molecular orbital (HOMO) and the lowest-unoccupied molecular orbital (LUMO) of iridium-based iTMCs to generate NIR emission. We describe a series of novel ionic iridium complexes with very small energy gaps, namely NIR1-NIR6, in which 2,3-diphenylbenzo[g]quinoxaline moieties mainly take charge of the HOMO energy levels and 2,2'-biquinoline, 2-(quinolin-2-yl)quinazoline, and 2,2'-bibenzo[d]thiazole moieties mainly control the LUMO energy levels. All the complexes exhibited NIR phosphorescence, with emission maxima up to 850 nm, and have been applied as components in LECs, showing a maximum external quantum efficiency (EQE) of 0.05 % in the EL devices. By using a host-guest emissive system, with the iridium complex RED as the host and the complex NIR3 or NIR6 as guest, the highest EQE of the LECs can be further enhanced to above 0.1 %.

Monolithic integration of GaN-based light-emitting diodes and metal-oxide-semiconductor field-effect transistors: reply.

We present some comments to the paper "Monolithic integration of GaN-based light-emitting diodes and metal-oxide-semiconductor field-effect transistors: comment," [Opt. Express22, A1589 (2014)].

Speckle reduction using deformable mirrors with diffusers in a laser pico-projector.

We propose a design for speckle reduction in a laser pico-projector adopting diffusers and deformable mirrors. This research focuses on speckle noise suppression by changing the angle of divergence of the diffuser. Moreover, the speckle contrast value can be further reduced by the addition of a deformable mirror. The speckle reduction ability obtained using diffusers with different divergence angles is compared. Three types of diffuser designs are compared in the experiments. For Type 1 which uses a circular symmetric diffuser the speckle contrast value can be decreased to 0.0264. For Type 2, the speckle contrast value can be reduced to 0.0267 because of the inclusion of an elliptical distribution diffuser. With Type 3 which includes a combination of the circular distribution diffuser and elliptical distribution diffuser, the speckle contrast value can be reduced to 0.0236. For all three types, the speckle contrast value is lower than 0.05. Under this speckle value, the speckle phenomenon is invisible to the human eye.

Monolithic integration of GaN-based light-emitting diodes and metal-oxide-semiconductor field-effect transistors.

In this study, we report a novel monolithically integrated GaN-based light-emitting diode (LED) with metal-oxide-semiconductor field-effect transistor (MOSFET). Without additionally introducing complicated epitaxial structures for transistors, the MOSFET is directly fabricated on the exposed n-type GaN layer of the LED after dry etching, and serially connected to the LED through standard semiconductor-manufacturing technologies. Such monolithically integrated LED/MOSFET device is able to circumvent undesirable issues that might be faced by other kinds of integration schemes by growing a transistor on an LED or vice versa. For the performances of resulting device, our monolithically integrated LED/MOSFET device exhibits good characteristics in the modulation of gate voltage and good capability of driving injected current, which are essential for the important applications such as smart lighting, interconnection, and optical communication.

Experimental observation of extremely weak optical scattering from an interlocking carbon nanotube array.

We experimentally demonstrate a nearly wavelength-independent optical reflection from an extremely rough carbon nanotube sample. The sample is made of a vertically aligned nanotube array, is a super dark material, and exhibits a near-perfect blackbody emission at T=450 K-600 K. No other material exhibits such optical properties, i.e., ultralow reflectance accompanied by a lack of wavelength scaling behavior. This observation is a result of the lowest ever measured reflectance (R=0.0003) of the sample over a broad infrared wavelength of 3 µm < λ < 13 µm. This discovery may be attributed to the unique interlocking surface of the nanotube array, consisting of both a global, large scale and a short-range randomness.

Experimental realization of plasmonic filters for multispectral and dual-polarization optical detection.

We report the design and implementation of a new class of plasmonic filters that are both wavelength and polarization selective. The plasmonic filter consists of a five-layer metallic photonic crystal structure and operates inside the photonic bandgap regime. We show that by manipulating the middle layer geometry alone, it is possible to tune the Fabry-Perot resonance over a broad spectral range (lambda=1.25to1.63 microm) and in a monolithic fashion. Furthermore, we show that the resonance has a definite polarization character that is determined by the orientation of the first layer grating. The plasmonic filter may be integrated with an array of photodetectors for high-throughput spectral and polarimetric imaging applications.

Highly Plasmonic Titanium Nitride by Room-Temperature Sputtering.

Titanium nitride (TiN) has recently emerged as an attractive alternative material for plasmonics. However, the typical high-temperature deposition of plasmonic TiN using either sputtering or atomic layer deposition has greatly limited its potential applications and prevented its integration into existing CMOS device architectures. Here, we demonstrate highly plasmonic TiN thin films and nanostructures by a room-temperature, low-power, and bias-free reactive sputtering process. We investigate the optical properties of the TiN films and their dependence on the sputtering conditions and substrate materials. We find that our TiN possesses one of the largest negative values of the real part of the dielectric function as compared to all other plasmonic TiN films reported to date. Two-dimensional periodic arrays of TiN nanodisks are then fabricated, from which we validate that strong plasmonic resonances are supported. Our room-temperature deposition process can allow for fabricating complex plasmonic TiN nanostructures and be integrated into the fabrication of existing CMOS-based photonic devices to enhance their performance and functionalities.

A curvature-tunable random laser.

The application of random lasers has been restricted due to the absence of a well-defined resonant cavity, as the lasing action mainly depends on multiple light scattering induced by intrinsic disorders of the laser medium to establish the required optical feedback that hence increases the difficulty in efficiently tuning and modulating random lasing emissions. This study investigated whether the transport mean free path of emitted photons within disordered scatterers composed of ZnO nanowires is tunable by a curvature bending applied to the flexible polyethylene terephthalate (PET) substrate underneath, thereby creating a unique light source that can be operated above and below the lasing threshold for desirable spectral emissions. For the first time, the developed curvature-tunable random laser is implemented for in vivo biological imaging with much lower speckle noise compared to the non-lasing situation through simple mechanical bending, which is of great potential for studying the fast-moving physiological phenomenon such as blood flow patterns in mouse ear skin. It is expected that the experimental demonstration of the curvature-tunable random laser can provide a new route to develop disorder-based optoelectronic devices.

Tuning the Color Temperature of White-Light-Emitting Electrochemical Cells by Laser-Scanning Perovskite-Nanocrystal Color Conversion Layers.

The development of white-light-emitting electrochemical cells (LECs) has attracted great attention owing to their numerous advantages. Recently, perovskite materials have also shown many outstanding optoelectronic properties in light absorption and emission, and hence they are suitable for serving as the color conversion layers (CCLs) in solid-state white-light-emitting diodes (LEDs). Here, white LECs were fabricated by integrating non-doped blue-green LECs with CCLs made of a single composition of perovskite nanocrystal (NCs). Moreover, the correlated color temperatures (CCTs) of the white LECs can be tuned by modifying the optical properties of the perovskite NCs, in the same way as so as the color conversion properties of CCLs are tuned, through laser scan. By controlling the laser power, scanning number, and duty cycle of the scanned grating patterns on perovskite-NC CCLs, the CCTs of the white LECs can be tuned from 2502 K to nearly 4300 K. Since this method is much different from that used with conventional CCLs, which use multiple compositions of perovskite NCs to produce white light, the inherent anion-exchange issue of perovskite NCs can be avoided.

Flexible random lasers with tunable lasing emissions.

In this study, we experimentally demonstrated a flexible random laser fabricated on a polyethylene terephthalate (PET) substrate with a high degree of tunability in lasing emissions. Random lasing oscillation arises mainly from the resonance coupling between the emitted photons of gain medium (Rhodamine 6G, R6G) and the localized surface plasmon (LSP) of silver nanoprisms (Ag NPRs), which increases the effective cross-section for multiple light scattering, thus stimulating the lasing emissions. More importantly, it was found that the random lasing wavelength is blue-shifted monolithically with the increase in bending strains exerted on the PET substrate, and a maximum shift of ∼15 nm was achieved in the lasing wavelength, when a 50% bending strain was exerted on the PET substrate. Such observation is highly repeatable and reversible, and this validates that we can control the lasing wavelength by simply bending the flexible substrate decorated with the Ag NPRs. The scattering spectrum of the Ag NPRs was obtained using a dark-field microscope to understand the mechanism for the dependence of the wavelength shift on the exerted bending strains. As a result, we believe that the experimental demonstration of tunable lasing emissions based on the revealed structure is expected to open up a new application field of random lasers.

Visible three-dimensional metallic photonic crystal with non-localized propagating modes beyond waveguide cutoff.

We report experimental realization of a 5-layer three-dimensional (3D) metallic photonic crystal structure that exhibits characteristics of a 3D complete bandgap extending from near-infrared down to visible wavelength at around 650 nm. The structure also exhibits a new kind of non-localized passband mode in the infrared far beyond its metallic waveguide cutoff. This new passband mode is drastically different from the well-known defect mode due to point or line defects. Three-dimensional finite-difference-time-domain simulations were carried out and the results suggest that the passband modes are due to intra-structure resonances.

Laser-Scanned Programmable Color Temperature of Electroluminescence from White Light-Emitting Electrochemical Cells.

Recently, the control of correlated color temperature (CCT) of artificial solid-state white-light sources starts to attract more attention since CTs affect human physiology and health profoundly. In this work, we proposed and demonstrated a method that can widely tune the CCTs of electroluminescence (EL) from white-light-emitting electrochemical cells (LECs) by employing plasmonic filters. These integrated on-chip plasmonic filters are composed of semicontinuous thin Ag film or Ag nanoparticles (NPs) both included in the indium tin oxide anode contact, which have different characteristics of plasmonic resonant absorptions that can tune the EL spectra of white LECs. The CCTs of EL from white LECs integrated with semicontinuous thin Ag film and randomly distributed Ag NPs are 5778 and 2350 K, respectively. A commercially available laser scanning system was used to locally thermal anneal the semicontinuous thin Ag film to form the randomly distributed Ag NPs on the scanned areas. Hence, these two kinds of filters can be integrated on the same chip of white LEC, giving more freedom to control the CCTs of white EL and more potential applications. In addition, the laser scanning system used here is quite often used in display manufactures so that our proposed method can be immediately adopted by the light-emitting diode industry.

Enhancing UV-emissions through optical and electronic dual-function tuning of Ag nanoparticles hybridized with n-ZnO nanorods/p-GaN heterojunction light-emitting diodes.

ZnO nanorods (NRs) and Ag nanoparticles (NPs) are known to enhance the luminescence of light-emitting diodes (LEDs) through the high directionality of waveguide mode transmission and efficient energy transfer of localized surface plasmon (LSP) resonances, respectively. In this work, we have demonstrated Ag NP-incorporated n-ZnO NRs/p-GaN heterojunctions by facilely hydrothermally growing ZnO NRs on Ag NP-covered GaN, in which the Ag NPs were introduced and randomly distributed on the p-GaN surface to excite the LSP resonances. Compared with the reference LED, the light-output power of the near-band-edge (NBE) emission (ZnO, λ = 380 nm) of our hybridized structure is increased almost 1.5-2 times and can be further modified in a controlled manner by varying the surface morphology of the surrounding medium of the Ag NPs. The improved light-output power is mainly attributed to the LSP resonance between the NBE emission of ZnO NRs and LSPs in Ag NPs. We also observed different behaviors in the electroluminescence (EL) spectra as the injection current increases for the treatment and reference LEDs. This observation might be attributed to the modification of the energy band diagram for introducing Ag NPs at the interface between n-ZnO NRs and p-GaN. Our results pave the way for developing advanced nanostructured LED devices with high luminescence efficiency in the UV emission regime.

Enhanced external quantum efficiency in GaN-based vertical-type light-emitting diodes by localized surface plasmons.

Enhancement of the external quantum efficiency of a GaN-based vertical-type light emitting diode (VLED) through the coupling of localized surface plasmon (LSP) resonance with the wave-guided mode light is studied. To achieve this experimentally, Ag nanoparticles (NPs), as the LSP resonant source, are drop-casted on the most top layer of waveguide channel, which is composed of hydrothermally synthesized ZnO nanorods capped on the top of GaN-based VLED. Enhanced light-output power and external quantum efficiency are observed, and the amount of enhancement remains steady with the increase of the injected currents. To understand the observations theoretically, the absorption spectra and the electric field distributions of the VLED with and without Ag NPs decorated on ZnO NRs are determined using the finite-difference time-domain (FDTD) method. The results prove that the observation of enhancement of the external quantum efficiency can be attributed to the creation of an extra escape channel for trapped light due to the coupling of the LSP with wave-guided mode light, by which the energy of wave-guided mode light can be transferred to the efficient light scattering center of the LSP.

Strong light concentration at the subwavelength scale by a metallic hole-array structure.

A metallic two-dimensional hole-array (2DHA) sample is successfully fabricated and its transmission property measured at mid-infrared wavelengths (lambda ~ 1.5-20 microm). At the plasmonic resonance, the 2DHA sample exhibits a normal incidence transmittance of 80% at lambda = 7.6 microm. This corresponds to more than twice as much light that is transmitted as it impinges directly on the holes at the maxima of transmittance. This exceedingly large enhancement is attributed to a strong plasmonic resonance and an effective light concentration through an ultrathin metal film of 50 nm. This advancement will pave the way to a much enhanced infrared detection using a simple and compact 2DHA architecture.

Experimental observation of an extremely dark material made by a low-density nanotube array.

An ideal black material absorbs light perfectly at all angles and over all wavelengths. Here, we show that low-density vertically aligned carbon nanotube arrays can be engineered to have an extremely low index of refraction, as predicted recently by theory [Garcia-Vidal, F. J.; Pitarke, J. M.; Pendry, J. B. Phys. Rev. Lett. 1997, 78, 4289-4292] and, combined with the nanoscale surface roughness of the arrays, can produce a near-perfect optical absorption material. An ultralow diffused reflectance of 1 x 10(-7) measured from such arrays is an order-of-magnitude lower compared to commercial low-reflectance standard carbon. The corresponding integrated total reflectance of 0.045% from the nanotube arrays is three times lower than the lowest-ever reported values of optical reflectance from any material, making it the darkest man-made material ever.