Achieving balanced charge transport is crucial for high-performance quantum-dot light-emitting diodes (QLEDs), yet it remains a significant challenge. This issue is notably evident when using high-mobility metal oxides, such as ZnO and SnO2 nanoparticles, as electron transport layers (ETLs), due to their excessive electron mobility which leads to a severe mismatch with most organic hole transport layers (HTLs). Consequently, the balanced charge injection and high efficiency in conventional QLEDs have been largely confined to high-mobility HTLs like poly(9,9-dioctyl-fluorene-co-N-(4-butylphenyl) diphenylamine) (TFB). In this study, we present a universal strategy to precisely tune the electron mobility of SnO2 nanocrystals through controlled Zn2+ doping concentration. This approach enables synergistic matching with a range of commonly used HTLs, achieving a near-ideal charge balance across all systems. As a result, we fabricated high-performance QLEDs with universal HTL compatibility, where all optimized devices exhibited a maximum external quantum efficiency (EQE) exceeding 27%. Importantly, the positive aging effect commonly observed in ZnMgO-based devices is completely eliminated in all our SnO2-based QLEDs. This work provides a general and universal ETL materials for fabricating highly efficient and stable QLEDs compatible with diverse hole transport materials without the need to consider their hole mobility.
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Chiral polar metal halides can generate spontaneous polarization, endowing them with potential for self-driven circularly polarized light (CPL) detection. However, most chiral metal halides crystallize in non-polar space groups and cannot generate spontaneous polarization, making efficient self-driven CPL detection difficult. In this work, for the first time, we propose a strategy to induce spontaneous polarization into non-polar chiral halides by introducing free halogens into the halide lattice via a solvothermal method. We find that this strategy not only breaks the intrinsic symmetry of non-polar R/S-MPZPbBr4 and transforms it into R/S-MPZPbBr4·0.5Br2 with the polar space group C2, but also induces larger octahedral distortion, which enhances the circular dichroism anisotropy factor (gCD) by 8 times. Benefiting from spontaneous polarization and the enhanced gCD, R/S-MPZPbBr4·0.5Br2 exhibits an anomalous photovoltaic effect of 3.8 V under zero bias and enables efficient self‑driven CPL detection, with an anisotropic response factor (gres) as high as 0.61. Our work opens a new pathway for designing chiral metal halides for self‑driven CPL detection.
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Chiral organic-inorganic hybrid halides show significant potential for applications in circularly polarized photodetection, chiral-induced spin selectivity effects (CISS), and nonlinear optics. However, the widespread use of toxic lead element poses environmental concerns, hindering the further applications. Herein, we synthesized a zero-dimensional (0D) lead-free chiral antimony-based halide (R/S-MBA)4Sb2Br10 with the coexistence of polarity and crystallographic chirality. The halides exhibit unique magneto-chiroptical effects due to the field-effect-induced fine-tuning of exciton energy, which is the first observation in chiral antimony-based halides. Furthermore, owing to its significant spontaneous polarization (5.0 μC/cm2) and optical chirality (gCD = 0.0018), (R/S-MBA)4Sb2Br10 halide exhibits excellent performance in self-powered circularly polarized photodetection, nonlinear optics, and CISS effects. The self-powered photodetector demonstrates high sensitivity with distinguishable factors (gres = 0.53/−0.51 @ 0 V) and broad spectral response. The single crystal (R/S-MBA)4Sb2Br10 also exhibits a high second-harmonic polarization response asymmetry factor (gSHG-CD = 0.98/−0.70) and strong second-harmonic generation intensity. These performances are among the best reported for chiral halides. Our research not only sheds new light on the investigation of magneto-chiroptical phenomena, but also marks a significant advancement in realizing high-sensitivity circularly polarized light detection within the realm of lead-free polar materials.
Zero-dimensional metal halides are of unique structures and tunable photoluminescence properties, showing great potential applications such as light-emitting diodes (LEDs) and sensing. Herein, we successfully synthesized Cu+ doped (MA)2ZnCl4 metal halides by a slow evaporation solvent method. The introduction of Cu+ results in sky-blue self-trapped exciton emission in (MA)2ZnCl4 at 486 nm at room temperature, and a photoluminescence quantum yield is as high as 54.9%. Interestingly, at low temperatures, Cu+-doped (MA)2ZnCl4 exhibits two emission peaks located at 482 and 605 nm, respectively. This temperature-dependent dual emission indicates two excited state structures that exist on the triplet excited-state potential energy surface. In addition, the temperature sensor we fitted has good performance (Sr = 1.65 %·K−1), which is the first attempt in Cu+ doped Zn-based metal halides. Our work enriches the family of sky-blue metal halides and provides a promising strategy for building sky-blue LEDs.
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