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Light emitting diodes (LEDs) have wide applications from fullcolor displays to solid‐state lighting. Numerous types of luminescent materials have been explored for LEDs, ranging from inorganic semiconductors to metal complexes and quantum dots. Despite the rapid pace of development, LEDs have not achieved their full potentials in terms of performance and cost efficiency. Identifying new eco‐friendly materials for LEDs is of great interest. Recently, metal halide perovskites and perovskite‐related hybrid materials have emerged as new generation luminescent materials with unique optoelectronic properties. Here, some of our recent development of LEDs based on metal halide perovskites and perovskite‐related materials will be discussed.more » « less
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A computational investigation is presented, in conjunction with synthesis and experimental characterization, into the structural, electronic, and optical properties of layered two‐dimensional organic lead bromide perovskites. Materials based on the chiral (R/S)‐4‐fluoro‐α‐methylbenzylammonium (R/S‐FMBA), which have been shown to lead to bright room‐temperature circularly polarized luminescence, are contrasted with the similar achiral 4‐fluorobenzylammonium (FBA). Using density functional theory (DFT) with van der Waals (vdW) corrections, relaxed structures (compared with X‐ray diffraction, XRD) and optical absorption spectra (compared with experiments) are studied, as well as band structure and orbital character of transitions. A Python code is developed and provided to calculate octahedral distortions and compare DFT and XRD results, finding that vdW corrections are important for accuracy and that DFT overestimates octahedral tilt angles. (FMBA)2PbBr4shows among the largest tilt angle differences (often termed ) reported, 14°–15°, indicating strong inversion symmetry‐breaking, which enables its chiral emission. A large resulting Dresselhaus spin‐splitting effect is found. The lowest‐energy optical transitions involve the perovskite only and are polarized within the layer. This work furthers understanding of structure‐property relations with applications to optoelectronics and spintronics.more » « less
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Abstract Low dimensional (LD) organic metal halide hybrids (OMHHs) have recently emerged as new generation functional materials with exceptional structural and property tunability. Despite the remarkable advances in the development of LD OMHHs, optical properties have been the major functionality extensively investigated for most of LD OMHHs developed to date, while other properties, such as magnetic and electronic properties, remain significantly under‐explored. Here, we report for the first time the characterization of the magnetic and electronic properties of a 1D OMHH, organic‐copper (II) chloride hybrid (C8H22N2)Cu2Cl6. Owing to the antiferromagnetic coupling between Cu atoms through chloride bridges in 1D [Cu2Cl62−]∞chains, (C8H22N2)Cu2Cl6is found to exhibit antiferromagnetic ordering with a Néel temperature of 24 K. The two‐terminal (2T) electrical measurement on a (C8H22N2)Cu2Cl6single crystal reveals its insulating nature. This work shows the potential of LD OMHHs as a highly tunable quantum material platform for spintronics.more » « less
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Abstract 0D organic metal halide hybrids (OMHHs) have recently emerged as a new generation of scintillation materials, due to their high luminescence quantum efficiency, sensitivity, stability, and cost‐effectiveness. While numerous 0D OMHH scintillators have been developed to date, most of them are based on solution grown single crystals that require time‐consuming synthesis and are limited in size. Here, high‐performance X‐ray scintillators based on facile solution processed 0D OMHH amorphous films are reported for the first time. By reacting triphenyl(9‐phenyl‐9H‐carbazol‐3‐yl) phosphonium bromide (TPPcarzBr) with manganese bromide (MnBr2), 0D (TPPcarz)₂MnBr₄ amorphous films can be prepared via solution processing with mild thermal annealing, which exhibits green photoluminescence with an emission maximum ≈517 nm and a photoluminescence quantum efficiency of ≈87%. The X‐ray scintillation of 0D (TPPcarz)₂MnBr₄ amorphous films is characterized to exhibit a light yield of 44600 photon MeV−1and an outstanding linearity with a low limit of detection of 32.42 nGyairs−1over a wide range of X‐ray dose rates. The versatile processability of 0D (TPPcarz)₂MnBr₄ is illustrated with remarkable recyclability, high cost‐effectiveness, and scalability for large‐scale production. By taking advantage of the amorphous nature of newly designed OMHHs, the approach opens up new opportunities for developing high‐performance, solution‐processable scintillators.more » « less
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Abstract Electrically driven light‐emitting diodes (ED LEDs) based on 3D metal halide perovskites have seen remarkable advancements during the past decade. However, the highest‐performing devices are largely based on lead‐containing 3D perovskites, presenting two key challenges – toxicity and stability – that must be addressed for commercialization. Reducing structural dimensionality and incorporating non‐lead metals present promising pathways to address these issues. Although research on ED LEDs based on low‐dimensional, lead‐free metal halides (LD LFMHs) is growing, their performance still significantly lags behind that of 3D lead halide perovskites. This review seeks to deliver a comprehensive overview of ED LEDs based on LD LFMHs, covering a brief history of their development, methods for material synthesis, luminescence mechanisms, and applications in electroluminescent devices. It also examines current challenges and proposes practical strategies to enhance device performance, with the goal of inspiring further progress in the field.more » « less
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Organic metal halide hybrids with low-dimensional structures at the molecular level have received great attention recently for their exceptional structural tunability and unique photophysical properties. Here we report for the first time the synthesis and characterization of a one-dimensional (1D) organic metal halide hybrid, which contains metal halide nanoribbons with a width of three octahedral units. It is found that this material with a chemical formula C 8 H 28 N 5 Pb 3 Cl 11 shows a dual emission with a photoluminescence quantum efficiency (PLQE) of around 25%. Photophysical studies and density functional theory (DFT) calculations suggest the coexisting of delocalized free excitons and localized self-trapped excitons in metal halide nanoribbons leading to the dual emission.more » « less
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