Efficient Photothermal Catalytic Oxidation Enabled by Three-Dimensional Nanochannel Substrates.

Photothermal catalysis exhibits promising prospects to overcome the shortcomings of high-energy consumption of traditional thermal catalysis and the low efficiency of photocatalysis. However, there is still a challenge to develop catalysts with outstanding light absorption capability and photothermal conversion efficiency for the degradation of atmospheric pollutants. Herein, we introduced the Co3O4 layer and Pt nanoclusters into the three-dimensional (3D) porous membrane through the atomic layer deposition (ALD) technique, leading to a Pt/Co3O4/AAO monolithic catalyst. The 3D ordered nanochannel structure can significantly enhance the solar absorption capacity through the light-trapping effect. Therefore, the embedded Pt/Co3O4 catalyst can be rapidly heated and the O2 adsorbed on the Pt clusters can be activated to generate sufficient O2- species, exhibiting outstanding activity for the diverse VOCs (toluene, acetone, and formaldehyde) degradation. Optical characterization and simulation calculation confirmed that Pt/Co3O4/AAO exhibited state-of-the-art light absorption and a notable localized surface plasmon resonance (LSPR) effect. In situ diffuse reflectance infrared Fourier transform spectrometry (in situ DRIFTS) studies demonstrated that light irradiation can accelerate the conversion of intermediates during toluene and acetone oxidation, thereby inhibiting byproduct accumulation. Our finding extends the application of AAO's optical properties in photothermal catalytic degradation of air pollutants.

Improving the Operational Lifetime of Metal-Halide Perovskite Light-Emitting Diodes with Dimension Control and Ligand Engineering.

Perovskite light-emitting diodes (LEDs) have emerged as one of the most propitious candidates for next-generation lighting and displays, with the highest external quantum efficiency (EQE) of perovskite LEDs already surpassing the 20% milestone. However, the further development of perovskite LEDs primarily relies on addressing operational instability issues. This Perspective examines some of the key factors that impact the lifetime of perovskite LED devices and some representative reports on recent advancements aimed at improving the lifetime. Our analysis underscores the significance of "nano" strategies in achieving long-term stable perovskite LEDs. Significant efforts must be directed toward proper device encapsulation, perovskite material passivation, interfacial treatment to address environment-induced material instability, bias-induced phase separation, and ion migration issues.

Geometric Shape Recognition with an Ultra-High Density Perovskite Nanowire Array-Based Artificial Vision System.

Artificial vision systems (AVS) have potential applications in visual prosthetics and artificially intelligent robotics, and they require a preprocessor and a processor to mimic human vision. Halide perovskite (HP) is a promising preprocessor and processor due to its excellent photoresponse, ubiquitous charge migration pathways, and innate hysteresis. However, the material instability associated with HP thin films hinders their utilization in physical AVSs. Herein, we have developed ultrahigh-density arrays of robust HP nanowires (NWs) rooted in a porous alumina membrane (PAM) as the active layer for an AVS. The NW devices exhibit gradual photocurrent change, responding to changes in light pulse duration, intensity, and number, and allow contrast enhancement of visual inputs with a device lifetime of over 5 months. The NW-based processor possesses temporally stable conductance states with retention >105 s and jitter <10%. The physical AVS demonstrated 100% accuracy in recognizing different shapes, establishing HP as a reliable material for neuromorphic vision systems.

High-efficiency, flexible and large-area red/green/blue all-inorganic metal halide perovskite quantum wires-based light-emitting diodes.

Metal halide perovskites have shown great promise as a potential candidate for next-generation solid state lighting and display technologies. However, a generic organic ligand-free and antisolvent-free solution method to fabricate highly efficient full-color perovskite light-emitting diodes has not been realized. Herein, by utilizing porous alumina membranes with ultra-small pore size as templates, we have successfully fabricated crystalline all-inorganic perovskite quantum wire arrays with ultrahigh density and excellent uniformity, using a generic organic ligand-free and anti-solvent-free solution method. The quantum confinement effect, in conjunction with the high light out-coupling efficiency, results in high photoluminescence quantum yield for blue, sky-blue, green and pure-red perovskite quantum wires arrays. Consequently, blue, sky-blue, green and pure-red LED devices with spectrally stable electroluminescence have been successfully fabricated, demonstrating external quantum efficiencies of 12.41%, 16.49%, 26.09% and 9.97%, respectively, after introducing a dual-functional small molecule, which serves as surface passivation and hole transporting layer, and a halide vacancy healing agent.

Self-Generated Buried Submicrocavities for High-Performance Near-Infrared Perovskite Light-Emitting Diode.

Embedding submicrocavities is an effective approach to improve the light out-coupling efficiency (LOCE) for planar perovskite light-emitting diodes (PeLEDs). In this work, we employ phenethylammonium iodide (PEAI) to trigger the Ostwald ripening for the downward recrystallization of perovskite, resulting in spontaneous formation of buried submicrocavities as light output coupler. The simulation suggests the buried submicrocavities can improve the LOCE from 26.8 to 36.2% for near-infrared light. Therefore, PeLED yields peak external quantum efficiency (EQE) increasing from 17.3% at current density of 114 mA cm-2 to 25.5% at current density of 109 mA cm-2 and a radiance increasing from 109 to 487 W sr-1 m-2 with low rolling-off. The turn-on voltage decreased from 1.25 to 1.15 V at 0.1 W sr-1 m-2. Besides, downward recrystallization process slightly reduces the trap density from 8.90 × 1015 to 7.27 × 1015 cm-3. This work provides a self-assembly method to integrate buried output coupler for boosting the performance of PeLEDs.

Three-Dimensional Nanopillar Arrays-Based Efficient and Flexible Perovskite Solar Cells with Enhanced Stability.

Perovskite nanopillars (PNPs) are propitious candidates for solar irradiation harvesting and are potential alternatives to thin films in flexible photovoltaics. To realize efficient daily energy output, photovoltaics must absorb sunlight over a broad range of incident angles and wavelengths congruent with the solar spectrum. Herein, we report highly periodic three-dimensional (3D) PNP-based flexible photovoltaics possessing a core-shell structure. The vertically aligned PNP arrays demonstrate up to 95.70% and 75.10% absorption at peak and under an incident angle of 60°. The efficient absorption and the orthogonal carrier collection facilitate an external quantum efficiency of 84.0%-89.18% for broadband wavelength. PNPs have been successfully implemented in flexible solar cells. The porous alumina membrane protects PNPs against water and oxygen intrusion and thereby imparts robustness to photovoltaic devices. Meanwhile, the excellent tolerance to mechanical stress/strain enables our unique PNP-based device to provide efficient solar-to-electricity conversion while undergoing mechanical bending.

Non-invasive and quantitive analysis of flatfoot based on ultrasound.

Flatfoot is a common foot deformity that seriously affects the quality of life. The aim of this study is to develop an accurate and noninvasive method for the diagnosis of flatfoot based on B-mode ultrasound. In this study, 51 patients (the flatfoot group) and 43 healthy subjects (the control group) were included. The plantar fascia angle, a new measurement for use in the diagnosis of flatfoot is proposed, as determined using B-mode ultrasound. For comparison, the calcaneal pitch angle and medial cuneiform height were also measured using lateral X-radiography, based on traditional diagnostic methods. The intraclass correlation values of the plantar fascia angle, the calcaneal pitch angle, and the medial cuneiform height were all more than 0.95, and there is a moderate correlation (r = 0.51) between the medial cuneiform height and the calcaneal pitch angle, and an excellent correlation (r = 0.85) between the plantar fascia angle and the calcaneal pitch angle. The optimal cutoff value, sensitivity, and specificity for medial cuneiform height in flatfoot diagnosis were 12.8 mm, 93.0%, and 54.9%, respectively. The optimal cutoff value, sensitivity, and specificity for plantar fascia angle in flatfoot diagnosis were 9.8°, 97.7%, and 94.1%, respectively. The proposed plantar fascia angle has good sensitivity and specificity in diagnosing flatfoot, therefore supplying a new approach for the noninvasive diagnosis of flatfoot.

Compound dietary fiber and high-grade protein diet improves glycemic control and ameliorates diabetes and its comorbidities through remodeling the gut microbiota in mice.

Dietary intervention with a low glycemic index and full nutritional support is emerging as an effective strategy for diabetes management. Here, we found that the treatment of a novel compound dietary fiber and high-grade protein diet (CFP) improved glycemic control and insulin resistance in streptozotocin-induced diabetic mice, with a similar effect to liraglutide. In addition, CFP treatment ameliorated diabetes-related metabolic syndromes, such as hyperlipidemia, hepatic lipid accumulation and adipogenesis, systemic inflammation, and diabetes-related kidney damage. These results were greatly associated with enhanced gut barrier function and altered gut microbiota composition and function, especially those bacteria, microbial functions, and metabolites related to amino acid metabolism. Importantly, no adverse effect of CFP was found in our study, and CFP exerted a wider arrange of protection against diabetes than liraglutide. Thereby, fortification with balanced dietary fiber and high-grade protein, like CFP, might be an effective strategy for the management and treatment of diabetes.

Uncooled self-powered hemispherical biomimetic pit organ for mid- to long-infrared imaging.

Infrared vision is highly desirable for applications in multifarious fields. Of the few species with this visual capability, snakes have exceptional infrared perception with the assistance of pit organs. Inspired by the pit organ design we present here a hemispherical biomimetic infrared imaging device. The devices use high-density ionic thermoelectric polymer nanowire arrays that serve as the sensing nerve cells. The individual nanowires exhibit notable voltage response to temperature variation in test objects. An infrared sensor array with 625 pixels on the hemispherical substrate is successfully demonstrated with an ultrawide field of view up to 135°. The device can image body temperature objects without a cooling system and external power supply. This work opens up opportunities for the design and fabrication of bioinspired infrared imaging devices based on emerging ionic thermoelectric materials.

Strongly Quantum-Confined Perovskite Nanowire Arrays for Color-Tunable Blue-Light-Emitting Diodes.

Color tunability of perovskite light-emitting diodes (PeLEDs) by mixed halide compositional engineering is one of the primary intriguing characteristics of PeLEDs. However, mixed halide PeLEDs are often susceptible to color red-shifting caused by halide ion segregation. In this work, strongly quantum-confined perovskite nanowires (QPNWs) made of CsPbBr3 are grown in nanoporous anodic alumina templates using a closed space sublimation process. By tuning the pore size with atomic layer deposition, QPNWs with a diameter of 6.6 to 2.8 nm have been successfully obtained, with continuous tunable photoluminescence emission color from green (512 nm) to pure blue (467 nm). To better understand the photophysics of QPNWs, carrier dynamics and the benefit of alumina passivation are studied and discussed in detail. Eventually, PeLEDs using various diameters of CsPbBr3 QPNWs are successfully fabricated with cyan color (492 nm) PeLEDs, achieving a record high 7.1% external quantum efficiency (EQE) for all CsPbBr3-based cyan color PeLEDs. Sky blue (481 nm) and pure blue (467 nm) PeLEDs have also been successfully demonstrated, respectively. The work here demonstrates a different approach to achieve quantum-confined one-dimensional perovskite structures and color-tunable PeLEDs, particularly blue PeLEDs.

Image processing with a multi-level ultra-fast three dimensionally integrated perovskite nanowire array.

Besides its ubiquitous applications in optoelectronics, halide-perovskites (HPs) have also carved a niche in the domain of resistive switching memories (Re-RAMs). However owing to the material and electrical instability challenges faced by HP thin-films, rarely perovskite Re-RAMs are used to experimentally demonstrate data processing which is a fundamental requirement for neuromorphic applications. Here, for the first time, lead-free, ultrahigh density HP nanowire (NW) array Re-RAM has been utilized to demonstrate image processing via design of convolutional kernels. The devices exhibited superior switching characteristics including a high endurance of 5 × 106 cycles, an ultra-fast erasing and writing speed of 900 ps and 2 ns, respectively, and a retention time >5 × 104 s for the resistances. The work is bolstered by an in-depth mechanistic study and first-principles simulations which provide evidence of electrochemical metallization triggering the switching. Employing the robust multi-level switching behaviour, image processing functions of embossing, outlining and sharpening were successfully implemented.

Vertical Heterogeneous Integration of Metal Halide Perovskite Quantum-Wires/Nanowires for Flexible Narrowband Photodetectors.

Charge collection narrowing (CCN) has been reported to be an efficient strategy to achieve optical filter-free narrowband photodetection (NPD) with metal halide perovskite (MHP) single crystals. However, the necessity of utilizing thick crystals in CCN limits their applications in large scale, flexible, self-driven, and high-performance optoelectronics. Here, for the first time, we fabricate vertically integrated MHP quantum wire/nanowire (QW/NW) array based photodetectors in nanoengineered porous alumina membranes (PAMs) showing self-driven broadband photodetection (BPD) and NPD capability simultaneously. Two cutoff detection edges of the NPDs are located at around 770 and 730 nm, with a full-width at half-maxima (fwhm) of around 40 nm. The optical bandgap difference between the NWs and the QWs, in conjunction with the high carrier recombination rate in QWs, contributes to the intriguing NPD performance. Thanks to the excellent mechanical flexibility of the PAMs, a flexible NPD is demonstrated with respectable performance. Our work here opens a new pathway to design and engineer a nanostructured MHP for novel color selective and full color sensing devices.

Three-dimensional perovskite nanowire array-based ultrafast resistive RAM with ultralong data retention.

Resistive random access memories (Re-RAMs) have transpired as a foremost candidate among emerging nonvolatile memory technologies with a potential to bridge the gap between the traditional volatile and fast dynamic RAMs and the nonvolatile and slow FLASH memories. Here, we report electrochemical metallization (ECM) Re-RAMs based on high-density three-dimensional halide perovskite nanowires (NWs) array as the switching layer clubbed between silver and aluminum contacts. NW Re-RAMs made of three types of methyl ammonium lead halide perovskites (MAPbX3; X = Cl, Br, I) have been explored. A trade-off between device switching speed and retention time was intriguingly found. Ultrafast switching speed (200 ps) for monocrystalline MAPbI3 and ~7 × 109 s ultralong extrapolated retention time for polycrystalline MAPbCl3 NW devices were obtained. Further, first-principles calculation revealed that Ag diffusion energy barrier increases when lattice size shrinks from MAPbI3 to MAPbCl3, culminating in the trade-off between the device switching speed and retention time.

Down-Scalable and Ultra-fast Memristors with Ultra-high Density Three-Dimensional Arrays of Perovskite Quantum Wires.

With strikingly high speed, data retention ability and storage density, resistive RAMs have emerged as a forerunning nonvolatile memory. Here we developed a Re-RAM with ultra-high density array of monocrystalline perovskite quantum wires (QWs) as the switching matrix with a metallic silver conducting pathway. The devices demonstrated high ON/OFF ratio of ∼107 and ultra-fast switching speed of ∼100 ps which is among the fastest in literature. The devices also possess long retention time of over 2 years and record high endurance of ∼6 × 106 cycles for all perovskite Re-RAMs reported. As a concept proof, we have also successfully demonstrated a flexible Re-RAM crossbar array device with a metal-semiconductor-insulator-metal design for sneaky path mitigation, which can store information with long retention. Aggressive downscaling to ∼14 nm lateral dimension produced an ultra-small cell effectively having 76.5 nm2 area for single bit storage. Furthermore, the devices also exhibited unique optical programmability among the low resistance states.

Optically tunable ultra-fast resistive switching in lead-free methyl-ammonium bismuth iodide perovskite films.

Resistive RAMs (Re-RAMs) have come to the fore as a rising star among the next generation non-volatile memories with fast operational speed, excellent endurance and prolonged data retention capabilities. Re-RAMs are being profusely used as storage and processing modules in neuromorphic hardware and high frequency switches in radio-frequency (RF) circuits. Owing to its intrinsic hysteresis and abundance of charge migration pathways, lead halide perovskites have emerged as a promising switching medium in Re-RAMs besides their ubiquitous usage in optoelectronic devices. Here, we adopted a lead-free eco-friendly methyl-ammonium bismuth iodide (MA3Bi2I9) perovskite (prepared by solvent-free engineering) as the switching medium sandwiched between copper (Cu) and indium doped tin oxide (ITO) electrodes. The devices exhibited a 104 high ON/OFF ratio that provided a large window for the multi-bit data storage in a single cell with good accuracy. Robust endurance of 1730 cycles and good data retention ability of >3 × 105 s were also observed. Careful switching speed measurements showed the devices can operate with an ultra-fast speed of 10 ns for writing and erasing respectively. The devices responded to light illumination and the prolonged retention of the opto-electrically tuned resistance states paved the way for image memorization.

A biomimetic eye with a hemispherical perovskite nanowire array retina.

Human eyes possess exceptional image-sensing characteristics such as an extremely wide field of view, high resolution and sensitivity with low aberration1. Biomimetic eyes with such characteristics are highly desirable, especially in robotics and visual prostheses. However, the spherical shape and the retina of the biological eye pose an enormous fabrication challenge for biomimetic devices2,3. Here we present an electrochemical eye with a hemispherical retina made of a high-density array of nanowires mimicking the photoreceptors on a human retina. The device design has a high degree of structural similarity to a human eye with the potential to achieve high imaging resolution when individual nanowires are electrically addressed. Additionally, we demonstrate the image-sensing function of our biomimetic device by reconstructing the optical patterns projected onto the device. This work may lead to biomimetic photosensing devices that could find use in a wide spectrum of technological applications.

Three-Dimensional Perovskite Nanophotonic Wire Array-Based Light-Emitting Diodes with Significantly Improved Efficiency and Stability.

Hybrid perovskites have emerged as promising candidates for highly efficient light-emitting diodes in the past few years due to their excellent crystallinity, high color purity, wide-range bandgap tunability, and solution processability. However, the reported device external quantum efficiency has not reached the level on par with that of conventional inorganic and organic light-emitting diodes. Moreover, device stability still needs substantial improvement. In this work, we demonstrate the fabrication of perovskite nanophotonic wire array-based light-emitting diodes with a capillary-effect-assisted template method. Compared with the planar control device, the nanostructured device demonstrates 45% improvement of external quantum efficiency from 11% to 16% owing to substantial enhancement on device light extraction efficiency verified by optical modeling. Intriguingly, it is also discovered that the nanostructured device possesses 3.89 times lifetime compared to the planar control device, due to effective template passivation. The results here have clearly shown that with a proper photonic device structure design, both the device performance and lifetime can be significantly improved.

Room-Temperature Sputtered SnO2 as Robust Electron Transport Layer for Air-Stable and Efficient Perovskite Solar Cells on Rigid and Flexible Substrates.

Extraordinary photovoltaic performance and intriguing optoelectronic properties of perovskite solar cells (PSCs) have aroused enormous interest from both academic research and photovoltaic (PV) industry. In order to bring PSC technology from laboratory to market, material stability, device flexibility, and scalability are important issues to address for vast production. Nevertheless, PSCs are still primarily prepared by solution methods which limit film scalability, while high-temperature processing of metal oxide electron transport layer (ETL) makes PSCs costly and incompatible with flexible substrates. Here, we demonstrate rarely-reported room-temperature radio frequency (RF) sputtered SnO2 as a promising ETL with suitable band structure, high transmittance, and excellent stability to replace its solution-processed counterpart. Power conversion efficiencies (PCEs) of 12.82% and 5.88% have been achieved on rigid glass substrate and flexible PEN substrate respectively. The former device retained 93% of its initial PCE after 192-hour exposure in dry air while the latter device maintained over 90% of its initial PCE after 100 consecutive bending cycles. The result is a solid stepping stone toward future PSC all-vapor-deposition fabrication which is being widely used in the PV industry now.

Increasing Photoluminescence Quantum Yield by Nanophotonic Design of Quantum-Confined Halide Perovskite Nanowire Arrays.

High-photoluminescence quantum yield (PLQY) is required to reach optimal performance in solar cells, lasers, and light-emitting diodes (LEDs). Typically, PLQY can be increased by improving the material quality to reduce the nonradiative recombination rate. It is in principle equally effective to improve the optical design by nanostructuring a material to increase light out-coupling efficiency (OCE) and introduce quantum confinement, both of which can increase the radiative recombination rate. However, increased surface recombination typically minimizes nanostructure gains in PLQY. Here a template-guided vapor phase growth of CH3NH3PbI3 (MAPbI3) nanowire (NW) arrays with unprecedented control of NW diameter from the bulk (250 nm) to the quantum confined regime (5.7 nm) is demonstrated, while simultaneously providing a low surface recombination velocity of 18 cm s-1. This enables a 56-fold increase in the internal PLQY, from 0.81% to 45.1%, and a 2.3-fold increase in OCEy to increase the external PLQY by a factor of 130, from 0.33% up to 42.6%, exclusively using nanophotonic design.

Efficient metal halide perovskite light-emitting diodes with significantly improved light extraction on nanophotonic substrates.

Metal halide perovskite has emerged as a promising material for light-emitting diodes. In the past, the performance of devices has been improved mainly by optimizing the active and charge injection layers. However, the large refractive index difference among different materials limits the overall light extraction. Herein, we fabricate efficient methylammonium lead bromide light-emitting diodes on nanophotonic substrates with an optimal device external quantum efficiency of 17.5% which is around twice of the record for the planar device based on this material system. Furthermore, optical modelling shows that a high light extraction efficiency of 73.6% can be achieved as a result of a two-step light extraction process involving nanodome light couplers and nanowire optical antennas on the nanophotonic substrate. These results suggest that utilization of nanophotonic structures can be an effective approach to achieve high performance perovskite light-emitting diodes.