Angew Chem Int Ed Engl
December 2024
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.
View Article and Find Full Text PDFMetal halide perovskites and perovskite-related organic metal halide hybrids (OMHHs) have recently emerged as a new class of luminescent materials for light emitting diodes (LEDs), owing to their unique and remarkable properties, including near-unity photoluminescence quantum efficiencies, highly tunable emission colors, and low temperature solution processing. While substantial progress has been made in developing monochromatic LEDs with electroluminescence across blue, green, red, and near-infrared regions, achieving highly efficient and stable white electroluminescence from a single LED remains a challenging and under-explored area. Here, a facile approach to generating white electroluminescence is reported by combining narrow sky-blue emission from metal halide perovskites and broadband orange/red emission from zero-dimensional (0D) OMHHs.
View Article and Find Full Text PDFLow 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 (CHN)CuCl.
View Article and Find Full Text PDFThe expanding applications of X-ray scintillation across various areas, from healthcare to security detection call for the development of new-generation scintillators that offer enhanced sensitivity, efficiency, and versatility. Here, we report for the first time the use of organic metal halide complexes with aggregation-induced emission (AIE) for X-ray scintillation, which can be facilely synthesized and processed in the solution phase. By reacting an AIE organic molecule, 4-(4-(diphenylamino) phenyl)-1-(propyl)-pyridinium (TPA-PD) with zinc chloride (ZnCl) in solution at room temperature, an organic metal halide complex, (TPA-PD)ZnCl, is produced with a high synthetic yield of 87%.
View Article and Find Full Text PDFScintillators, one of the essential components in medical imaging and security checking devices, rely heavily on rare-earth-containing inorganic materials. Here, a new type of organic-inorganic hybrid scintillators containing earth abundant elements that can be prepared via low-temperature processes is reported. With room temperature co-crystallization of an aggregation-induced emission (AIE) organic halide, 4-(4-(diphenylamino) phenyl)-1-(propyl)-pyrindin-1ium bromide (TPA-PBr), and a metal halide, zinc bromide (ZnBr ), a zero-dimensional (0D) organic metal halide hybrid (TPA-P) ZnBr with a yellowish-green emission peaked at 550 nm has been developed.
View Article and Find Full Text PDFOrganic 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 CHNPbCl shows a dual emission with a photoluminescence quantum efficiency (PLQE) of around 25%.
View Article and Find Full Text PDFZero-dimensional (0D) organic metal halide hybrids (OMHHs) have recently emerged as a new class of light emitting materials with exceptional color tunability. While near-unity photoluminescence quantum efficiencies (PLQEs) are routinely obtained for a large number of 0D OMHHs, it remains challenging to apply them as emitter for electrically driven light emitting diodes (LEDs), largely due to the low conductivity of wide bandgap organic cations. Here, the development of a new OMHH, triphenyl(9-phenyl-9H-carbazol-3-yl) phosphonium antimony bromide (TPPcarzSbBr ), as emitter for efficient LEDs, which consists of semiconducting organic cations (TPPcarz ) and light emitting antimony bromide anions (Sb Br ), is reported.
View Article and Find Full Text PDFFLASH radiation therapy is a novel technique combining ultra-high dose rates (UHDR) with very short treatment times to strongly decrease normal tissue toxicity while preserving the anti-tumoral effect. However, the radiobiological mechanisms and exact conditions for obtaining the FLASH-effect are still under investigation. There are strong indications that parameters defining the beam structure, such as dose per pulse, instantaneous dose rate and pulse repetition frequency (PRF) are of importance.
View Article and Find Full Text PDFIonically bonded organic metal halide hybrids have emerged as versatile multicomponent material systems exhibiting unique and useful properties. The unlimited combinations of organic cations and metal halides lead to the tremendous structural diversity of this class of materials, which could unlock many undiscovered properties of both organic cations and metal halides. Here we report the synthesis and characterization of a series benzoquinolinium (BZQ) metal halides with a general formula (BZQ)PbX (X = Cl, Br), in which metal halides form a unique two-dimensional (2D) structure.
View Article and Find Full Text PDFLow-dimensional hybrid metal halides are emerging as a highly promising class of single-component white-emitting materials for their unique broadband emission from self-trapped excitons (STEs). Despite substantial progress in the development of these metal halides, many challenges remain to be addressed to obtain a better fundamental understanding of the structure-property relationship and realize the full potentials of this class of materials. Here, via pressure regulation, a near 100% photoluminescence quantum yield (PLQY) of broadband emission is achieved in a corrugated 1D hybrid metal halide C N H Pb Br , which possesses a highly distorted structure with an initial PLQY of 10%.
View Article and Find Full Text PDFCathepsin L (CTL) is a cysteine protease demonstrating upregulated activity in many disease states. Overlapping substrate specificity makes selective detection of CTL activity difficult to parse from that of its close homologue CTV and the ubiquitous CTB. Current probes of CTL activity have limited applications due to either poor contrast or extra assay steps required to achieve selectivity.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
February 2021
Surface passivation of perovskite solar cells (PSCs) using a low-cost industrial organic pigment quinacridone (QA) is presented. The procedure involves solution processing a soluble derivative of QA, N,N-bis(tert-butyloxycarbonyl)-quinacridone (TBOC-QA), followed by thermal annealing to convert TBOC-QA into insoluble QA. With halide perovskite thin films coated by QA, PSCs based on methylammonium lead iodide (MAPbI ) showed significantly improved performance with remarkable stability.
View Article and Find Full Text PDFThe fabrication of efficient and spectrally stable pure-blue perovskite light-emitting diodes (LEDs) has been elusive and remains of great interest. Herein, we incorporate diammonium salts into quasi-2D perovskite precursors for phase control of multiple quantum well structures to yield tunable and efficient emission in the blue region. With detailed characterizations and computational studies, we show that in situ passivation by the diammonium salts effectively modifies the surface energies of quasi-2D phases and inhibits the growth of low-band gap quasi-2D and 3D phases.
View Article and Find Full Text PDFThe photophysical tuning is reported for a series of tetraphenylphosphonium (TPP) metal halide hybrids containing distinct metal halides, TPP MX (MX =SbCl , MnCl , ZnCl , ZnCl Br , ZnBr ), from efficient phosphorescence to ultralong afterglow. The afterglow properties of TPP cations could be suspended for the hybrids containing low band gap emissive metal halide species, such as SbCl and MnCl , but significantly enhanced for the hybrids containing wide band gap non-emissive ZnCl . Structural and photophysical studies reveal that the enhanced afterglow is attributed to stronger π-π stacking and intermolecular electronic coupling between TPP cations in TPP ZnCl than in the pristine organic ionic compound TPPCl.
View Article and Find Full Text PDFLow-dimensional perovskite-related metal halides have emerged as a new class of light-emitting materials with tunable broadband emission from self-trapped excitons (STEs). Although various types of low-dimensional structures have been developed, fundamental understating of the structure-property relationships for this class of materials is still very limited, and further improvement of their optical properties remains greatly important. Here, we report a significant pressure-induced photoluminescence (PL) enhancement in a one-dimensional hybrid metal halide CNHPbBr, and the underlying mechanisms are investigated using in situ experimental characterization and first-principles calculations.
View Article and Find Full Text PDFBinuclear platinum(II) complexes with strong Pt-Pt interactions are an interesting class of luminescent materials, of which photophysical properties could be controlled via multiple ways through organic ligands and Pt-Pt distance. While a number of binuclear platinum(II) complexes have been developed with tunable emissions, achieving high photoluminescence quantum efficiency (PLQE) remains challenging and of great interest. Here we report the synthesis and characterization of a series of binuclear 2,4-difluorophenylpyridine platinum(II) complexes bridged by thiazol-2-thiolate ligands with different bulkiness.
View Article and Find Full Text PDFScintillation based X-ray detection has received great attention for its application in a wide range of areas from security to healthcare. Here, we report highly efficient X-ray scintillators with state-of-the-art performance based on an organic metal halide, ethylenebis-triphenylphosphonium manganese (II) bromide ((CHP)MnBr), which can be prepared using a facile solution growth method at room temperature to form inch sized single crystals. This zero-dimensional organic metal halide hybrid exhibits green emission peaked at 517 nm with a photoluminescence quantum efficiency of ~ 95%.
View Article and Find Full Text PDFMetal halide perovskite nanocrystals (NCs) have emerged as new-generation light-emitting materials with narrow emissions and high photoluminescence quantum efficiencies (PLQEs). Various types of perovskite NCs, e.g.
View Article and Find Full Text PDFZero-dimensional (0D) organic metal halide hybrids, in which organic and metal halide ions cocrystallize to form neutral species, are a promising platform for the development of multifunctional crystalline materials. Herein we report the design, synthesis, and characterization of a ternary 0D organic metal halide hybrid, (HMTA) PbMn Sn Br , in which the organic cation N-benzylhexamethylenetetrammonium (HMTA , C H N ) cocrystallizes with PbBr , MnBr , and SnBr . The wide band gap of the organic cation and distinct optical characteristics of the three metal bromide anions enabled the single-crystalline "host-guest" system to exhibit emissions from multiple "guest" metal halide species simultaneously.
View Article and Find Full Text PDFACS Appl Mater Interfaces
January 2020
The interfaces between perovskite and charge transport layers greatly impact the device efficiency and stability of perovskite solar cells (PSCs). Inserting an ultrathin wide-band-gap layer between perovskite and hole transport layers (HTLs) has recently been shown as an effective strategy to enhance device performance. Herein, a small amount of an organic halide salt, ,'-dimethylethylene-1,2-diammonium iodide, is used to create two-dimensional (2D)-three-dimensional (3D) heterojunctions on MAPbI thin film surfaces by facile solution processing.
View Article and Find Full Text PDFOrganometal halide perovskite materials, in particular colloidal perovskite nanocrystals (NCs), have been investigated extensively as next-generation light-emitting materials. However, producing highly efficient and stable perovskite thin films from colloidal NCs is not trivial, as dissociation of surfactants often occurs during the thin-film formation. Here, we demonstrate a facile solution-processing approach to prepare perovskite nanocomposite thin films by using phosphonium as the capping ligand for methylammonium lead bromide (MAPbBr) NCs.
View Article and Find Full Text PDFThe rich chemistry of metal halide perovskites has enabled various methods of band structure control and surface passivation. Here we report a highly facile and efficient post-treatment approach for precise color tuning of cesium lead halide perovskite nanocrystals (NCs) with enhanced stability. By utilizing a special multifunctional organic ligand, triphenyl(9-phenyl-9H-carbazol-3-yl)phosphonium bromide (TPP-Carz), carbon-halide bond cleavage can be achieved to release halide ions from halogenated solvents in a controlled manner for color tuning of perovskite NCs via ion exchange.
View Article and Find Full Text PDFThe rich chemistry of organic-inorganic metal halide hybrids has enabled the development of a variety of crystalline structures with controlled morphological and molecular dimensionalities. Here we report for the first time a single crystalline assembly of metal halide clusters, (CNH)(PbCl)PbCl, in which lead chloride tetrahedrons (PbCl) and face-sharing lead chloride trimer clusters (PbCl) cocrystallize with organic cations (CNH) to form a periodical zero-dimensional (0D) structure at the molecular level. Blue light emission peaked at 470 nm with a photoluminescence quantum efficiency (PLQE) of around 83% was realized for this single crystalline hybrid material, which is attributed to the individual lead chloride clusters.
View Article and Find Full Text PDFACS Appl Mater Interfaces
September 2018
Here we report ultraviolet (UV)-pumped white-light-emitting diodes (WLEDs) with sunlike full spectrum emissions, by using a commercially available blue phosphor (BaMgAlO:Eu) and a series of broadband zero-dimensional (0D) organic metal halide hybrids as down conversion phosphors. By controlling the blend ratio of phosphors, we have achieved high-quality WLEDs with excellent general color rendering index (CRI R) of up to 99 and deep-red rendering index (R9) of up to 99. These WLEDs exhibiting white emissions with correlated color temperatures (CCTs) ranging from 3000 to 6000 K perfectly mimic sunlight at different times of day.
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