Embedding TiO2microspheres into the active layer as light scatterers in a perovskite photodetector to boost light harvesting.

Here, TiO2microspheres with particle sizes of 200-400 nm are embedded in p-i-n perovskite photodetectors, which are used as light scatterers. This approach was implemented to change the light transfer path in the perovskite layer, which gives the device higher photon-capture ability in a specific incident wavelength range. Compared with a pristine device, the photocurrent and responsivity of the device based on such a structure are obviously enhanced in the ranges of 560-610 nm and 730-790 nm. The photocurrent under 590 nm incident light wavelength illumination (light intensityP= 31.42µW·cm-2) increases from 1.45µA to 1.71µA, with an increase of 17.93%, and the responsivity reaches 0.305 A·W-1. In addition, the introduction of TiO2has no additional negative impact on the carrier extraction and the dark current. Also, the response time of the device did not deteriorate. Finally, the role of TiO2as light scatterers is further verified by embedding microspheres into mixed-halide perovskite devices.

Defect recombination suppression and carrier extraction improvement for efficient CsPbBr3/SnO2heterojunction photodetectors.

Perovskite materials with excellent optical and electronic properties have huge potential in the research field of photodetectors. Constructing heterojunctions and promoting carrier transportation are significant for the development of perovskite-based optoelectronics devices with high performances. Herein, we demonstrated a CsPbBr3/SnO2heterojunction photodetector and improved the device performances through post-annealing treatment of SnO2film. The results indicated that the electrical properties of SnO2films will make an important impact on carrier extraction, especially for type-II heterojunction. As the electrons transfer layer in CsPbBr3/SnO2type-II heterojunction, defects related to oxygen vacancy should be the key factor to affect carrier concentration, induce carriers' limitation and recombination rate. Under proper annealing temperature for SnO2layer, the recombination rate can decrease to 1.37 × 1021cm3s and the spectral responsivity will be highly increased. This work can enhance the understanding on the photoresponse of perovskite photodetectors, and will be helpful for the further optimization and design of optoelectronic devices based on the perovskite heterojunction.

MDACl2-Modified SnO2 Film for Efficient Planar Perovskite Solar Cells.

The electron transport layer (ETL) with excellent charge extraction and transport ability is one of the key components of high-performance perovskite solar cells (PSCs). SnO2 has been considered as a more promising ETL for the future commercialization of PSCs due to its excellent photoelectric properties and easy processing. Herein, we propose a facile and effective ETL modification strategy based on the incorporation of methylenediammonium dichloride (MDACl2) into the SnO2 precursor colloidal solution. The effects of MDACl2 incorporation on charge transport, defect passivation, perovskite crystallization, and PSC performance are systematically investigated. First, the surface defects of the SnO2 film are effectively passivated, resulting in the increased conductivity of the SnO2 film, which is conducive to electron extraction and transport. Second, the MDACl2 modification contributes to the formation of high-quality perovskite films with improved crystallinity and reduced defect density. Furthermore, a more suitable energy level alignment is achieved at the ETL/perovskite interface, which facilitates the charge transport due to the lower energy barrier. Consequently, the MDACl2-modified PSCs exhibit a champion efficiency of 22.30% compared with 19.62% of the control device, and the device stability is also significantly improved.

Sequential Processing Enables 17% All-Polymer Solar Cells via Non-Halogen Organic Solvent.

All-polymer solar cells (All-PSCs), whose electron donor and acceptors are both polymeric materials, have attracted great research attention in the past few years. However, most all-PSC devices with top-of-the-line efficiencies are processed from chloroform. In this work, we apply the sequential processing (SqP) method to fabricate All-PSCs from an aromatic hydrocarbon solvent, toluene, and obtain efficiencies up to 17.0%. By conducting a series of characterizations on our films and devices, we demonstrate that the preparation of SqP devices using toluene can effectively reduce carrier recombination, enhance carrier mobility and promote the fill factor of the device.

Revealing the Hidden Mechanism of Enhanced Responsivity of Doped p-i-n Perovskite Photodiodes via Coupled Opto-Electronic Model.

Organic-inorganic halide perovskites have demonstrated preeminent optoelectronic performance in recent years due to their unique material properties, and have shown great potential in the field of photodetectors. In this study, a coupled opto-electronic model is constructed to reveal the hidden mechanism of enhancing the performance of perovskite photodetectors that are suitable for both inverted and regular structure doped p-i-n perovskite photodiodes. Upon illumination, the generation rate of photogenerated carriers is calculated followed by carrier density distribution, which serves as a coupled joint to further analyze the recombination rate, electric field strength, and current density of carriers under different doping types and densities. Moreover, experiments were carried out in which the doping types and densities of the active layer were regulated by changing the precursor ratios. With optimal doping conditions, the inverted and regular perovskite photodiodes achieved an external quantum efficiency of 74.83% and 73.36%, and a responsivity of 0.417 and 0.404 A/W, respectively. The constructed coupled opto-electronic model reveals the hidden mechanism and along with the doping strategy, this study provides important guidance for further analysis and improvement of perovskite-based photodiodes.

Analyzing and modulating energy transfer in ternary-emissive system of quantum dot light-emitting diodes towards efficient emission.

The mechanisms for energy transfer including Förster resonance energy transfer (FRET) and radiative energy transfer in ternary-emissive system consists of blended-quantum dots (QDs, red-QDs blended with blue-QDs) emissive layer (EML) and blue-emissive hole-transport material that contained in quantum dot light-emitting diodes (QLEDs) are complicated. As the energy transfer could exhibit either positive or negative impact on QD's photoluminescence (PL) and electroluminescence (EL), it is important to analyze and modulate energy transfer in such ternary-emissive system to obtain high-efficiency QLEDs. In this work, we have demonstrated that proper B-QDs doping has a positive impact on R-QDs' PL and EL, where these improvements were attributed to the B-QDs' spacing effect on R-QDs which weakens homogeneous FRET among R-QDs and near 100% efficient heterogeneous FRET from B-QDs to R-QDs. With optimization based on the analysis of energy transfer, the PL quantum yield of blended-QDs (with R:B blending ratio of 90:10, in quality) film has been enhanced by 35% compared with that of unblended R-QDs film. Moreover, thanks to the spacing effect and high-efficiency FRET from B-QDs to R-QDs, the external quantum efficiency of QLEDs that integrate optimized blended-QDs (R:B=90:10) EML reaches 22.1%, which is 15% higher than that of the control sample (19.2%) with unblended R-QDs EML. This work provides a systematically analytical method to study the energy transfer in ternary-emissive system, and gives a valid reference for the analysis and development of the emerging QLEDs that with blended-QDs EML.

A Novel Upside-Down Thermal Annealing Method Toward High-Quality Active Layers Enables Organic Solar Cells with Efficiency Approaching 20.

The emerging non-fullerene acceptors with low voltage losses have pushed the power conversion efficiency of organic solar cells (OSCs) to ≈20% with auxiliary morphology optimization. Thermal annealing (TA), as the most widely adopted post-treatment method, has been playing an essential role in realizing the potential of various material systems. However, the procedure of TA, i.e., the way that TA is performed, is almost identical among thousands of OSC papers since ≈30 years ago other than changes in temperature and annealing time. Herein, a reverse thermal annealing (RTA) technique is developed, which can enhance the dielectric constant of active layer film, thereby producing a smaller Coulomb capture radius (14.93 nm), meanwhile, forming a moderate nano-scale phase aggregation and a more favorable face-on molecular stacking orientation. Thus, this method can reduce the decline in open circuit voltage of the conventional TA method by achieving decreased radiative (0.334 eV) and non-radiative (0.215 eV) recombination loss. The power conversion efficiency of the RTA PM6:L8-BO-X device increases to 19.91% (certified 19.42%) compared to the TA device (18.98%). It is shown that this method exhibits a superb universality in 4 other material systems, revealing its dramatic potential to be employed in a wide range of OSCs.

Performance Enhancement of Perovskite Quantum Dot Light-Emitting Diodes via Management of Hole Injection.

Poly(3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS) is widely used in optoelectronic devices due to its excellent hole current conductivity and suitable work function. However, imbalanced carrier injection in the PEDOT:PSS layer impedes obtaining high-performance perovskite light-emitting diodes (PeLEDs). In this work, a novel poly[(9,9-dioctylfluorenyl-2,7-diyl)-co-(4,40-(N-(p-butylphenyl))diphenylamine)] (TFB) is applied as the hole transport layers (HTLs) to facilitate the hole injection with cascade-like energy alignment between PEDOT:PSS and methylammonium lead tribromide (MAPbBr3) film. Our results indicate that the introduced TFB layer did not affect the surface morphology or lead to any additional surface defects of the perovskite film. Consequently, the optimal PeLEDs with TFB HTLs show a maximum current efficiency and external quantum efficiency (EQE) of 21.26 cd A-1 and 6.68%, respectively. Such EQE is 2.5 times higher than that of the control devices without TFB layers. This work provides a facile and robust route to optimize the device structure and improve the performance of PeLEDs.

Efficient All-Polymer Solar Cells with Sequentially Processed Active Layers.

In this work, we apply the sequential processing (SqP) method to address the relatively low electron mobility in recent all-polymer solar cells (all-PSCs) based on the polymerized small-molecule acceptor (PSMA). Compared to the blend-casting (BC) method, all-PSCs composed of PM6/PY-IT via the SqP method show boosted electron mobility and a more balanced charge carrier transport, which increases the FF of the SqP device and compensates for the short-circuit current loss, rendering comparable overall performance with the BC device. Through film-depth-dependent light absorption spectroscopy, we analyze the sub-layer absorption and exciton generation rate in the vertical direction of the device, and discuss the effect of the increased electron mobility on device performance, accordingly.

A ZIF-8-based multifunctional intelligent drug release system for chronic osteomyelitis.

Chronic osteomyelitis (COM) is an inflammatory bone disease caused by bacterial infection. Conventional treatment with antibiotics is prone to resistance and other side effects, and it is ineffective against inflammation caused by infection and bone loss. To treat COM comprehensively, based on the acidic microenvironment of osteomyelitis, we used ZIF-8 and celecoxib to construct a multifunctional intelligent drug release system with pH response effect, named CEL@ZIF-8. Material characterization revealed that celecoxib is successfully loaded into ZIF-8. Ion release and drug release experiments indicated that CEL@ZIF-8 can respond well to the pH and intelligently control the release of ions and drugs. Antibacterial assays manifested that CEL@ZIF-8 is able to inhibit the growth of bacteria significantly. In vitro cell experiments demonstrated that CEL@ZIF-8 can significantly up-regulate the expression of osteogenesis-related cytokines and down-regulate the levels of inflammatory factors. Studies verify that the novel drug release system possesses multiple functions: antibacterial, osteogenesis, anti-inflammatory and intelligent release, suggesting a tremendous clinical promise for the treatment of COM.

Efficient All-Polymer Solar Cells Enabled by Interface Engineering.

All-polymer solar cells (all-PSCs) are organic solar cells in which both the electron donor and the acceptor are polymers and are considered more promising in large-scale production. Thanks to the polymerizing small molecule acceptor strategy, the power conversion efficiency of all-PSCs has ushered in a leap in recent years. However, due to the electrical properties of polymerized small-molecule acceptors (PSMAs), the FF of the devices is generally not high. The typical electron transport material widely used in these devices is PNDIT-F3N, and it is a common strategy to improve the device fill factor (FF) through interface engineering. This work improves the efficiency of all-polymer solar cells through interfacial layer engineering. Using PDINN as the electron transport layer, we boost the FF of the devices from 69.21% to 72.05% and the power conversion efficiency (PCE) from 15.47% to 16.41%. This is the highest efficiency for a PY-IT-based binary all-polymer solar cell. This improvement is demonstrated in different all-polymer material systems.

Turing patterns with high-resolution formed without chemical reaction in thin-film solution of organic semiconductors.

Regular patterns can form spontaneously in chemical reaction-diffusion systems under non-equilibrium conditions as proposed by Alan Turing. Here, we found that regular patterns can be generated in uphill-diffusion solution systems without a chemical reaction process through both in-situ and ex-situ observations. Organic semiconductor solution is confined between two parallel plates with controlled micron/submicron-meter distance to minimize convection of the liquid and avoid spinodal precipitation at equilibrium. The solvent evaporation concentrates the solution gradually into an oversaturated non-equilibrium condition, under which a phase-transition occurs and ordered concentration-waves are generated. By proper tuning of the experimental parameter, multiple regular patterns with micro/nano-meter scaled features (line, square-grid, zig-zag, and fence-like patterns etc.) were observed. We explain the observed phenomenon as Turing-pattern generation resulted from uphill-diffusion and solution oversaturation. The generated patterns in the solutions can be condensed onto substrates to form structured micro/nanomaterials. We have fabricated organic semiconductor devices with such patterned materials to demonstrate the potential applications. Our observation may serve as a milestone in the progress towards a fundamental understanding of pattern formation in nature, like in biosystem, and pave a new avenue in developing self-assembling techniques of micro/nano structured materials.

Marked Efficiency Improvement of FAPb0.7Sn0.3Br3 Perovskite Light-Emitting Diodes by Optimization of the Light-Emitting Layer and Hole-Transport Layer.

Highly luminescent FAPb0.7Sn0.3Br3 nanocrystals with an average photoluminescence (PL) quantum yield of 92% were synthesized by the ligand-assisted reprecipitation method. The 41-nm-thick perovskite film with a smooth surface and strong PL intensity was proven to be a suitable luminescent layer for perovskite light-emitting diodes (PeLEDs). Electrical tests indicate that the double hole-transport layers (HTLs) played an important role in improving the electrical-to-optical conversion efficiency of PeLEDs due to their cascade-like level alignment. The PeLED based on poly[(9,9-dioctylfluorenyl-2,7-diyl)-co-(4,40-(N-(p-butylphenyl))-diphenylamine)] (TFB)/poly(9-vinylcarbazole) (PVK) double HTLs produced a high external quantum efficiency (EQE) of 9%, which was improved by approximately 10.9 and 5.14 times when compared with single HTL PVK or the TFB device, respectively. The enhancement of the hole transmission capacity by TFB/PVK double HTLs was confirmed by the hole-only device and was responsible for the dramatic EQE improvement.

Review for Rare-Earth-Modified Perovskite Materials and Optoelectronic Applications.

In recent years, rare-earth metals with triply oxidized state, lanthanide ions (Ln3+), have been demonstrated as dopants, which can efficiently improve the optical and electronic properties of metal halide perovskite materials. On the one hand, doping Ln3+ ions can convert near-infrared/ultraviolet light into visible light through the process of up-/down-conversion and then the absorption efficiency of solar spectrum by perovskite solar cells can be significantly increased, leading to high device power conversion efficiency. On the other hand, multi-color light emissions and white light emissions originated from perovskite nanocrystals can be realized via inserting Ln3+ ions into the perovskite crystal lattice, which functioned as quantum cutting. In addition, doping or co-doping Ln3+ ions in perovskite films or devices can effectively facilitate perovskite film growth, tailor the energy band alignment and passivate the defect states, resulting in improved charge carrier transport efficiency or reduced nonradiative recombination. Finally, Ln3+ ions have also been used in the fields of photodetectors and luminescent solar concentrators. These indicate the huge potential of rare-earth metals in improving the perovskite optoelectronic device performances.

Fabrication of patterned solid surfaces with highly controllable wettability.

Precisely controlling the wettability of a solid surface is vital for a wide range of applications such as control of liquid droplet motion, water collection and the directional transport of fluids. However, fabricating a large-area solid surface with highly controllable wettability in a low-cost way is still challenging. Here we present a cost-effective method to fabricate patterned solid surfaces with highly controllable wettability by combining chemical etching technique, chemical vapor deposition technique and laser direct writing technique. We experimentally demonstrated that the contact angle of water droplets on the patterned surfaces of a porous nanofilm fabricated using the presented fabrication method can be adjusted from 94.4° to 168.2° by changing the duty ratio of the periodic pattern on the patterned surfaces. Furthermore, we experimentally demonstrated that the contact angle of water droplets on the patterned surfaces is almost independent of the shape of the unit cell of the patterns. In addition, we propose an effective surface model to accurately calculate the contact angle of water droplets on patterned solid surfaces. Using the effective surface model, the wettability of a patterned solid surface can be precisely controlled by designing the duty ratio of its periodic patterns.

Magnon Torque Transferred into a Magnetic Insulator through an Antiferromagnetic Insulator.

Electrical spin-orbit torque (SOT) in magnetic insulators (MI) has been intensively studied due to its advantages in spin-orbitronic devices with ultralow energy consumption. However, the magnon torque in the MIs, which has the potential to further lower the energy consumption, still remains elusive. In this work, we demonstrate the efficient magnon torque transferred into an MI through an antiferromagnetic insulator. By fabricating a Pt/NiO/Tm3Fe5O12 heterostructure with different NiO thicknesses, we have systematically investigated the evolution of the transferred magnon torque. We show that the magnon torque efficiency transferred through the NiO into the MI can retain a high value (∼50%), which is comparable to the previous report for the magnon torque transferred into the metallic magnet. Our study manifests the feasibility of realizing the pure magnon-based spin-orbitronic devices with ultralow energy consumption and high efficiency.

Preparation of Aluminum Nanomesh Thin Films from an Anodic Aluminum Oxide Template as Transparent Conductive Electrodes.

We have employed anodic aluminum oxide as a template to prepare ultrathin, transparent, and conducting Al films with a unique nanomesh structure for transparent conductive electrodes. The anodic aluminum oxide template is obtained through direct anodization of a sputtered Al layer on a glass substrate, and subsequent wet etching creates the nanomesh metallic film. The optical and conductive properties are greatly influenced by experimental conditions. By tuning the anodizing time, transparent electrodes with appropriate optical transmittance and sheet resistance have been obtained. The results demonstrate that our proposed strategy can serve as a potential method to fabricate low-cost TCEs to replace conventional indium tin oxide materials.