Efficient Green Spin Light-Emitting Diodes Enabled by Ultrafast Energy- and Spin-Funneling in Chiral Perovskites.

Introducing molecular chirality into perovskite crystal structures has enabled the control of carrier spin states, giving rise to circularly polarized luminescence (CPL) in thin films and circularly polarized electroluminescence (CPEL) in LEDs. Spin-LEDs can be fabricated either through a spin-filtering layer enabled by chiral-induced spin selectivity or a chiral emissive layer. The former requires a high degree of spin polarization and a compatible spinterface for efficient spin injection, which might not be easily integrated into LEDs. Alternatively, a chiral emissive layer can also generate circularly polarized electroluminescence, but the efficiency remains low and the fundamental mechanism is elusive. In this work, we report an efficient green LED based on quasi-two-dimensional (quasi-2D) chiral perovskites as the emitting layer (EML), where CPEL is directly produced without separate carrier spin injection. The optimized chiral perovskite thin films exhibited strong CPL at 535 nm with a photoluminescence quantum yield (PLQY) of 91% and a photoluminescence dissymmetry factor (glum) of 8.6 × 10-2. Efficient green spin-LEDs were successfully demonstrated, with a large EL dissymmetry factor (gEL) of 7.8 × 10-2 and a maximum external quantum efficiency (EQE) of 13.5% at room temperature. Ultrafast transient absorption (TA) spectroscopic study shows that the CPEL is generated from a rapid energy transfer accompanied by spin transfer from 2D to 3D perovskites. Our study not only demonstrates a reliable approach to achieve high performance spin-LEDs but also reveals the fundamental mechanism of CPEL with an emissive layer of chiral perovskites.

Synergistic nucleation regulation using 4,4',4''-tris(carbazol-9-yl)-triphenylamine and moisture for stably air-processed high-performance perovskite photodetectors.

Perovskite photodetectors (PPDs) offer a promising solution with low cost and high responsivity, addressing the limitations of traditional inorganic photodetectors. However, there is still room for improvement in terms of the dark current and stability of air-processed PPDs. In this study, 4,4',4''-tris(carbazol-9-yl)-triphenylamine (TCTA) was utilized as a nucleation agent to enhance the quality of perovskite films. The synergistic effect of TCTA and moisture promotes rapid nucleation of PbI2-PbCl2, resulting in an increased nucleation rate and the elimination of pinholes in the film. By employing additive engineering, we obtained a PbI2-PbCl2 layer with high coverage, leading to a low density of traps in the corresponding perovskite film. Consequently, the modified PPD exhibits a remarkable reduction in dark current density by over one order of magnitude, reaching 2.4 × 10-10 A cm-2 at -10 mV, along with a large linear dynamic range (LDR) of 183 dB. Furthermore, the resulting PPD demonstrates remarkable stability, retaining 90% of the initial external quantum efficiency (EQE) value even after continuous operation for over 3200 hours. Owing to a fast response time in the nanosecond range, the PPD could convert modulated light signals into electrical signals at a speed of 588 Kbit s-1, highlighting the great potential in the field of optical communication.

Reblooming of the cis-Bis(2-phenylpyridine) Platinum(II) Complex: Synthesis Updating, Aggregation-Induced Emission, Electroluminescence, and Cell Imaging.

Studies on the syntheses, photophysical properties, and applications of cis-bis(2-phenylpyridine) platinum(II) complex (Pt(ppy)2) family are of great importance, but very limited progress has been achieved to date. Herein, a one-pot method was established for the syntheses of Pt(ppy)2-type complexes Pt-ppy and Pt-tBu. These two compounds were nonemissive in dilute solutions. However, they produced intense red and deep-red phosphorescence in the aggregation and film states, with lifetimes and quantum yields up to 1.92 µs and 70%, respectively, exhibiting unique aggregation-induced emission (AIE) characteristics. According to the experimental and theoretical studies, molecular configuration transformation (MCT) in the excited state may occur because of the d-d transition from the Pt center, causing nonradiative transitions in the solution. Nevertheless, the MCT would be largely restricted by the intermolecular interactions or rigid matrix, thereby enabling efficient phosphorescence in the aggregation state and in the PMMA films. Consequently, the AIE characteristics of Pt-ppy and Pt-tBu probably result from the restriction of molecular configuration transformation (RMCT). Due to the π-π and/or weak Pt-Pt interactions and the concentration-dependent emission characteristics, they emit deep-red and NIR emissions generated by excimer and/or MMLCT emitting species. Inspired by their AIE features, electroluminescence and cell imaging applications are explored. To the best of our knowledge, this is the first comprehensive study on the synthesis optimization, photophysical properties, AIE characteristics, and applications of the Pt(ppy)2-type complexes, which may rebloom the research studies on this type of Pt(II) complex family and provide valuable insights on the development of phosphorescent AIE metal-organic complexes.

Understanding the degradation mechanism of TTA-based blue fluorescent OLEDs by exciton dynamics and transient electroluminescence measurements.

The lifetime of blue organic light-emitting diodes (OLEDs) has always been a big challenge in practical applications. Blue OLEDs based on triplet-triplet annihilation (TTA) up-conversion materials have potential to achieve long lifetimes due to fusing two triplet excitons to one radiative singlet exciton, but there is a lack of an in-depth understanding of exciton dynamics on degradation mechanisms. In this work, we established a numerical model of exciton dynamics to study the impact factors in the stability of doped blue OLEDs based on TTA up-conversion hosts. By performing transient electroluminescence experiments, the intrinsic parameters related to the TTA up-conversion process of aging devices were determined. By combining the change of excess charge density in the emitting layer (EML) with aging time, it is concluded that the TTA materials are damaged by the excess electrons in the EML during ageing, which is the main degradation mechanism of OLEDs. This work provides a theoretical basis for preparing long-lifetime blue fluorescent OLEDs.

Synergistic Halide- and Ligand-Exchanges of All-Inorganic Perovskite Nanocrystals for Near-Unity and Spectrally Stable Red Emission.

All-inorganic perovskite nanocrystals (NCs) of CsPbX3 (X = Cl, Br, I) are promising for displays due to wide color gamut, narrow emission bandwidth, and high photoluminescence quantum yield (PLQY). However, pure red perovskite NCs prepared by mixing halide ions often result in defects and spectral instabilities. We demonstrate a method to prepare stable pure red emission and high-PLQY-mixed-halide perovskite NCs through simultaneous halide-exchange and ligand-exchange. CsPbBr3 NCs with surface organic ligands are first synthesized using the ligand-assisted reprecipitation (LARP) method, and then ZnI2 is introduced for anion exchange to transform CsPbBr3 to CsPbBrxI3-x NCs. ZnI2 not only provides iodine ions but also acts as an inorganic ligand to passivate surface defects and prevent ion migration, suppressing non-radiative losses and halide segregation. The luminescence properties of CsPbBrxI3-x NCs depend on the ZnI2 content. By regulating the ZnI2 exchange process, red CsPbBrxI3-x NCs with organic/inorganic hybrid ligands achieve near-unity PLQY with a stable emission peak at 640 nm. The CsPbBrxI3-x NCs can be combined with green CsPbBr3 NCs to construct white light-emitting diodes with high-color gamut. Our work presents a facile ion exchange strategy for preparing spectrally stable mixed-halide perovskite NCs with high PLQY, approaching the efficiency limit for display or lighting applications.

The Synergy of the Buried Interface Surface Energy and Temperature for Thermal Evaporated Perovskite Light-Emitting Diodes.

Multisource coevaporation is such a promising method for the preparation of perovskite films. However, there is limited research about the effects of the buried interface on thermal-evaporated perovskite light-emitting diodes (PeLEDs). In this study, the effects of buried interfaces on thermal-evaporated all-inorganic perovskite films are systematically investigated. It is found that the low-surface-energy buried interface promotes the formation of columnar grain by suppressing heterogeneous nucleation, and functional groups on the high-surface-energy interface have a significant effect on the actual element ratio of the film. The substrate temperature can affect the nucleation and film-formation kinetics of the columnar grains. As a result of the synergistic strategy, a peak external quantum efficiency (EQE) of 8.6% is achieved in the green PeLEDs with a stable emission peak at 516 nm, which is among the best thermal-evaporated PeLEDs reported. This work provides an insight into the preparation of perovskites by thermal evaporation and builds the groundwork for future studies.

Increasing the operating lifetime of green phosphorescent organic light emitting diodes by reducing charge accumulation at the interface.

The stability and degradation mechanism of phosphorescent organic light emitting diodes (OLEDs) has been an unresolved problem in the past decades. Here, we found that electron accumulation at the interface between the electron blocking layer and the emitting layer is one of the reasons for device degradation. By inserting a thin layer with a shallower LUMO level than that of the electron transporting layer between the emitting layer and the electron transporting layer, we successfully reduced the density of electrons at the interface and greatly improved the lifetime of the resulting green phosphorescent OLEDs. The half decay lifetime LT50 at the initial luminance of 1000 cd m-2 reached as high as 399 h, which is 1.7 times longer than that of the compared device without a thin layer.

Efficient Quasi-2D Perovskite Light-Emitting Diodes Enabled by Regulating Phase Distribution with a Fluorinated Organic Cation.

Metal halide perovskites have become a research highlight in the optoelectronic field due to their excellent properties. The perovskite light-emitting diodes (PeLEDs) have achieved great improvement in performance in recent years, and the construction of quasi-2D perovskites by incorporating large-size organic cations is an effective strategy for fabricating efficient PeLEDs. Here, we incorporate the fluorine meta-substituted phenethylammonium bromide (m-FPEABr) into CsPbBr3 to prepare quasi-2D perovskite films for efficient PeLEDs, and study the effect of fluorine substitution on regulating the crystallization kinetics and phase distribution of the quasi-2D perovskites. It is found that m-FPEABr allows the transformation of low-n phases to high-n phases during the annealing process, leading to the suppression of n = 1 phase and increasing higher-n phases with improved crystallinity. The rational phase distribution results in the formation of multiple quantum wells (MQWs) in the m-FPEABr based films. The carrier dynamics study reveals that the resultant MQWs enable rapid energy funneling from low-n phases to emission centers. As a result, the green PeLEDs achieve a peak external quantum efficiency of 16.66% at the luminance of 1279 cd m-2. Our study demonstrates that the fluorinated organic cations would provide a facile and effective approach to developing high-performance PeLEDs.

Ternary Electrical Memory Devices Based on Polycarbazole: SnO2 Nanoparticles Composite Material.

In this paper, a D-A polymer (PIB) containing carbazole as the donor group in the main chain and benzimidazole benzisoindolinone as the acceptor group was synthesized by Suzuki reaction. The Suzuki reaction, also known as the Suzuki coupling reaction, is a relatively new organic coupling reaction in which aryl or alkenyl boronic acids or boronic acid esters react with chlorine, bromine, iodoaromatic hydrocarbons or alkenes under the catalysis of zerovalent palladium complexes cross-coupling. A series of devices were fabricated by a spin-coating approach, and the devices all exhibited ternary resistance switching storage behavior. Among them, the composite device with the mass fraction of SnO2 NPs of 5 wt% has the best storage performance, with a threshold voltage of -0.4 V and a switching current ratio of 1:101.5:104.5. At the same time, the current of the device remained stable after a 3-h test. Furthermore, after 103 cycles, the current has no obvious attenuation. The device has good stability and continuity. Moreover, the conduction mechanism is further revealed. Inorganic nanoparticle composite devices have splendid memory performances and exhibit underlying application significance in storing data.

Ternary Flash Memory with a Carbazole-Based Conjugated Copolymer: WS2 Composites as Active Layers.

For nonvolatile memory devices, the design and synthesis of their substrate materials are very important. Due to the versatility and large-area fabrication of the low-temperature spin coating process, organic/inorganic nanomaterials as active layers of memory devices have been deeply studied. Inorganic nanoparticles can engage in interactions with polymers via external voltage. WS2 NPs have a large specific surface area and good conductivity. They can be used as the charge trap center in the active layer, which is conducive to the charge transfer in the active layer. Poly[2,7-9-(9-heptadecanyl)-9H-carbazole-co-benzo[4,5] imidazole[2,1-α] isoindol-11-one] (PIIO) was synthesized via the Suzuki coupling reaction. ITO/PIIO/Al and ITO/PIIO:WS2 NP/Al devices were prepared by the spin coating method and vacuum evaporation technology. All devices showed tristable switching behavior. The influence of the WS2 mass fraction on memory performance was studied. The device composite with 6 wt % WS2 NPs showed the best storage features. The OFF/ON1/ON2 current ratio was 1: 1.11 × 101: 2.03 × 104, and the threshold voltage Vth1/Vth2 was -0.60 V/-1.05 V. The device is steady for 12,000 s in three states-high-resistance state (HRS), intermediate state (IRS), and low-resistance state (LRS). After reading 3500 times, the switch-state current displayed no obvious attenuation. This work shows that the polymer and its composites have broad prospects in next-generation nonvolatile storage.

Low-dimensional phase suppression and defect passivation of quasi-2D perovskites for efficient electroluminescence and low-threshold amplified spontaneous emission.

Quasi-2D metal halide perovskites are promising candidates for light-emitting applications owing to their large exciton binding energy and strong quantum confinement effect. Usually, quasi-2D perovskites are composed of multiple phases with various numbers of layers (n) of metal halide octahedron sheets, enabling light emission from the lowest-bandgap phase by cascade energy transfer. However, the energy transfer processes are extremely sensitive to the phase distribution and trap density in the quasi-2D perovskite films, and the insufficient energy transfer between different-n phases and the defect-induced traps would result in nonradiative losses. Here, significantly reduced nonradiative losses in the quasi-2D perovskite films are achieved by tailoring the low-dimensional phase components and lowering the density of trap states. Butylammonium bromide (BABr) and potassium thiocyanate (KSCN) are employed to synergistically decrease the nonradiative recombination in the quasi-2D perovskite films of PEABr : CsPbBr3. The incorporation of BABr is found to suppress the formation of the n = 1 phase, while adding KSCN can further reduce the low-n phases, passivate the notorious defects and improve the alignment of the high-n phases. By incorporating appropriate contents of BABr and KSCN, the resultant quasi-2D perovskite films show high photoluminescence quantum yield (PLQY) and highly ordered crystal orientation, which enable not only the green light-emitting diodes (LEDs) with a high external quantum efficiency (EQE) of 16.3%, but also the amplified spontaneous emission (ASE) with a low threshold of 2.6 µJ cm-2. These findings provide a simple and effective strategy to develop high-quality quasi-2D perovskites for LED and laser applications.

Rearranging Low-Dimensional Phase Distribution of Quasi-2D Perovskites for Efficient Sky-Blue Perovskite Light-Emitting Diodes.

Metal halide perovskites have received much attention for their application in light-emitting diodes (LEDs) in the past several years. Rapid progress has been made in efficient green, red, and near-infrared perovskite LEDs. However, the development of blue perovskite LEDs is still lagging far behind. Here, we report efficient sky-blue perovskite LEDs by rearranging low-dimensional phase distribution in quasi-2D perovskites. We incorporated sodium ions into the mixed-Cl/Br quasi-2D perovskites with phenylethylammonium as the organic spacer and cesium lead halide as the inorganic framework. The inclusion of the sodium ion was found to significantly reduce the formation of the n = 1 phase, which was dominated by nonradiative transition, and increase the formation of other small-n phases for efficient exciton energy transfer. By managing the phase distribution, a maximum external quantum efficiency (EQE) of 11.7% was achieved in the sky-blue perovskite LED, with a stable emission peak at 488 nm. Further optimizing the phase distribution and film morphology with Pb content, we demonstrated the sky-blue devices with the average EQE approaching 10%. This strategy of engineering phase distribution of quasi-2D perovskites with a sodium ion could provide a useful way for the fabrication of high-performance blue perovskite LEDs.

Reducing greenhouse gas emissions and enhancing carbon and nitrogen conversion in food wastes by the black soldier fly.

Currently, sustainable utilisation, including recycling and valorisation, is becoming increasingly relevant in environmental management. The wastes bioconversion by the black soldier fly larva (BSFL) has two potential advantages: the larvae can convert the carbon and nitrogen in the biomass waste, and improve the properties of the substrate to reduce the loss of gaseous carbon and nitrogen. In the present study, the conversion rate of carbon, nitrogen and the emissions of greenhouse gases and NH3 during BSFL bio-treatment of food waste were investigated under different pH conditions. The results showed that the pH of the raw materials is a pivotal parameter affecting the process. The average wet weight of harvested BSFL was 13.26-95.28 mg/larva, with about 1.95-13.41% and 5.40-18.93% of recycled carbon and nitrogen from substrate at a pH from 3.0 to 11.0, respectively. Furthermore, pH is adversely correlated with CO2 emissions, but positively with NH3 emissions. Cumulative CO2, NH3, CH4 and N2O emissions at pH ranging from 3.0 to 11.0 were 88.15-161.11 g kg-1, 0.15-1.68 g kg-1, 0.19-2.62 mg kg-1 and 0.02-1.65 mg kg-1, respectively. Compared with the values in open composting, BSFL bio-treatment of food waste could lead greenhouse gas (especially CH4 and N2O) and NH3 emissions to decrease. Therefore, a higher pH value of the substrate can increase the larval output and help the mitigation of greenhouse gas emissions.

Effect of moisture content on greenhouse gas and NH3 emissions from pig manure converted by black soldier fly.

The effects of different moisture contents on greenhouse gas (GHG) emissions from pig manure (PM) digested by black soldier fly larvae (BSFL) as well as the accompanying changes of nitrogen and carbon contents in gaseous emissions and residues were studied. A mixture of PM and corncob at the ratio of 2.2:1 was prepared with a moisture content of 45%. Then, distilled water was added to adjust the moisture contents of the mixture to 55%, 65%, 75% and 85%, respectively. The prepared mixtures were digested by BSFL for eight days. The results indicated that BSFL could reduce CH4, N2O and NH3 emissions respectively by 72.63-99.99%, 99.68%-99.91% and 82.30-89.92%, compared with conventional composting, while CO2 emissions increased potentially due to BSFL metabolism. With increasing moisture content, the cumulative CH4 emissions increased, while cumulative NH3 emissions peaked at 55% moisture content and then decreased. Interestingly, the tendency of total cumulative CO2 emissions was consistent with that of the total weight of BSFL. The total GHG emissions were about only 1% those from of traditional composting at the optimum moisture content (75%), which was the most favorable for the growth of BSFL. The nitrogen and carbon contents of BSFL content in all treatments accounted for 1.03%-12.67% and 0.25%-4.68% of the initial contents in the raw materials, respectively. Moreover, the residues retained 71.12%-90.58% carbon and 67.91%-80.39% nitrogen of the initial raw materials. Overall, our results suggest that BSFL treatment is an environment-friendly alternative for decreasing CH4, N2O and NH3 emissions as well as reducing global warming potential (GWP).

Superior Efficiency and Low-Efficiency Roll-Off White Organic Light-Emitting Diodes Based on Multiple Exciplexes as Hosts Matched to Phosphor Emitters.

Based on exciplexes as hosts, the monochromatic organic light-emitting diodes (OLEDs) have achieved high power and external quantum efficiencies. However, the high-quality white OLEDs (WOLEDs) with high color rendering index (CRI) have the unsatisfactory efficiencies at high luminance, particularly in terms of power efficiency (PE), resulting in high energy consumption. Here, a new design concept using multiple exciplexes as hosts to match different phosphors has been demonstrated to develop high-performance WOLEDs. It can be seen that the resulting WOLEDs work at a low turn-on voltage of 2.3 V and exhibit the large forward-viewing PE and external quantum efficiency (EQE) of 79 lm W-1 and 22.5%, respectively, without light out-coupling techniques. Significantly, the PE and EQE still remain 48.0 lm W-1 and 21.4% at 1000 cd m-2, showing extremely low efficiency roll-off. The CRI is as high as 81. The keys to success are the selection of the different exciplex hosts matched to different phosphors and the reasonable arrangement of emissive layers, which are beneficial to regulate the exciton distribution and reduce the energy losses.

Strategic-tuning of radiative excitons for efficient and stable fluorescent white organic light-emitting diodes.

The emerging thermally activated delayed fluorescence materials have great potential for efficiencies in organic light-emitting diodes by optimizing molecular structures of the emitter system. However, it is still challenging in the device structural design to achieve high efficiency and stable device operation in white organic light-emitting diodes. Here we propose a universal design strategy for thermally activated delayed fluorescence emitter-based fluorescent white organic light-emitting diodes, establishing an advanced system of "orange thermally activated delayed fluorescence emitter sensitized by blue thermally activated delayed fluorescence host" combined with an effective exciton-confined emissive layer. Compared to reference single-layer and double-layer emissive devices, the external quantum efficiency improves by 31 and 45%, respectively, and device operational stability also shows nearly fivefold increase. Additionally, a detailed optical simulation for the present structure is made, indicating the validity of the design strategy in the fluorescent white organic light-emitting diodes.

Experimental realization of sequential weak measurements of non-commuting Pauli observables.

Sequential weak measurements of non-commuting observables are not only fundamentally interesting in terms of quantum measurement but also show potential in various applications. Previously reported methods, however, can only make limited sequential weak measurements experimentally. In this article, we propose the realization of sequential measurements of non-commuting Pauli observables and experimentally demonstrate for the first time the measurement of sequential weak values of three non-commuting Pauli observables using genuine single photons.

Controlling excimer formation in indolo[3,2,1-jk]carbazole/9H-carbazole based host materials for RGB PhOLEDs.

Three novel materials (5CzICz, Cz2ICz and Cz3ICz), based on the indolo[3,2,1-jk]carbazole and 9H-carbazole building blocks, with high triplet energies (E T > 2.80 eV) and good thermal stability (T g > 101 °C) were synthesized, characterized and applied as host materials in PhOLED devices. In course of the preparation of the materials, an improved protocol for the synthesis of the indolo[3,2,1-jk]carbazole moiety has been developed. The careful molecular design of the title compounds allowed to avoid excimer formation of the indolo[3,2,1-jk]carbazole subunits in thin films. Therefore, the improved molecular design broadened the applicability of indolo[3,2,1-jk]carbazole host materials and significantly enhanced the efficiency of PhOLED devices based on these derivatives compared to previously reported indolo[3,2,1-jk]carbazole based compounds. Accordingly, employing the newly developed materials red (CEmax: 32.7 cd A-1, PEmax: 31.0 lm W-1, EQEmax: 20.4%), green (CEmax: 81.0 cd A-1, PEmax: 87.4 lm W-1, EQEmax: 21.5%) and blue (CEmax: 35.5 cd A-1, PEmax: 39.9 lm W-1, EQEmax: 18.0%) PhOLED devices with a remarkably low efficiency roll-off at 1000 cd m-2 (Cz2ICz - red: 5%; green: 0%; blue: 6%) were fabricated.

In situ synthesis and macroscale alignment of CsPbBr3 perovskite nanorods in a polymer matrix.

We report an in situ catalyst-free strategy to synthesize inorganic CsPbBr3 perovskite nanorods in a polymer matrix (NRs-PM) with good dimensional control, outstanding optical properties and ultrahigh environmental stability. Polarization photoluminescence (PL) imaging with high spatial resolution was carried out for the first time on single nanorod (NR) and shows a relatively high local polarization ratio (∼0.4) consistent with theoretical predictions based on a dielectric contrast model. We further demonstrate that macroscale alignment of the CsPbBr3 nanorods can be achieved through mechanically stretching the NRs-PM films at elevated temperature, without deteriorating the optical quality of the NRs. A polarization ratio of 0.23 is observed for these aligned NRs-PM films, suggesting their potential as polarized down-converters to increase the light efficiency in liquid crystal display (LCD) backlights.

Extremely Low Roll-Off and High Efficiency Achieved by Strategic Exciton Management in Organic Light-Emitting Diodes with Simple Ultrathin Emitting Layer Structure.

Phosphorescent organic light-emitting diodes (OLEDs) possess the property of high efficiency but have serious efficiency roll-off at high luminance. Herein, we manufactured high-efficiency phosphorescent OLEDs with extremely low roll-off by effectively locating the ultrathin emitting layer (UEML) away from the high-concentration exciton formation region. The strategic exciton management in this simple UEML architecture greatly suppressed the exciton annihilation due to the expansion of the exciton diffusion region; thus, this efficiency roll-off at high luminance was significantly improved. The resulting green phosphorescent OLEDs exhibited the maximum external quantum efficiency of 25.5%, current efficiency of 98.0 cd A-1, and power efficiency of 85.4 lm W-1 and still had 25.1%, 94.9 cd A-1, and 55.5 lm W-1 at 5000 cd m-2 luminance, and retained 24.3%, 92.7 cd A-1, and 49.3 lm W-1 at 10 000 cd m-2 luminance, respectively. Compared with the usual structures, the improvement demonstrated in this work displays potential value in applications.