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All‐inorganic CsPbX3 (X = Cl, Br, or I) perovskite thin films are attractive emissive layers for high‐performance light‐emitting diodes (LEDs) due to their precisely tunable bandgaps, excellent color purities, good stabilities, and solution processabilities. However, the fabrication of high‐quality CsPbI3−xBrx thin films is very challenging because the crystal growth of mixed halide CsPbI3−xBrx is in low controllability. Herein, a synergetic regulation strategy using fluorine polymer (Poly(vinylidene fluoride‐co‐hexafluoropropylene)) and a small amino acid molecule (L‐Arginine) is developed to fabricate high‐quality CsPbI3−xBrx thin films for efficient pure red perovskite LEDs. In the fabricated CsPbI3−xBrx thin film, the fluorine polymer plays a crucial role in confining CsPbI3−xBrx crystal size at the nanoscale and the small amino acid molecule acts as a passivation agent to reduce the trap‐state density. Under this synergetic effect, a uniform CsPbI3−xBrx thin film with a high photoluminescence quantum yield up to 40% can be obtained to fabricate an efficient pure red perovskite LED with a maximum external quantum efficiency of 4.5% and a maximum brightness of 3100 cd m−2. The reported synergistic regulation strategy will open a new avenue to fabricate efficient pure color CsPbX3 perovskite LEDs. [ABSTRACT FROM AUTHOR]

The exploration of lead‐free halide perovskite nanocrystals (NCs) with intriguing optical properties is highly desirable owing to the toxicity and instability of lead halide perovskite NCs. Here, a new kind of uniform lead‐free double perovskite Cs2NaBiCl6 NCs are reported as versatile hosts to accommodate ionic dopants for improving optical properties especially the photoluminescence (PL). In contrast to the low deep‐blue PL with a quantum yield of only 1.7% of the as‐synthesized pristine Cs2NaBiCl6 NCs, the PL of the Cs2NaBiCl6 NCs can be impressively regulated and enhanced via doping Ag+, Mn2+, or Eu3+ ions in the double perovskite lattices. The femtosecond time‐resolved transient absorption spectroscopy is adopted to unravel the PL enhancement mechanism of the ion doping in the Cs2NaBiCl6 NCs. For the Ag+‐doping, the excitonic absorption energy of the Cs2NaBiCl6 NCs can be tuned from 3.82 to 3.48 eV with the significant improvement of the PL quantum yield (PLQY) from 1.7% to 20%. The Mn2+‐doped Cs2NaBiCl6 NCs show broad orange–red emission peak centered at 585 nm with a PLQY of 3%, owing to the 4T1→6A1 transition of octahedrally coordinated Mn2+. Eu3+‐doped Cs2NaBiCl6 NCs are endowed with strong Eu3+5D0→7FJ (J = 1, 2) orange–red emission at 591 and 615 nm. [ABSTRACT FROM AUTHOR]

Abstract: Aggregation‐induced emission (AIE) is an attractive phenomenon in which materials display strong luminescence in the aggregated solid states rather than in the conventional dissolved molecular states. However, highly luminescent inks based on AIE are hard to be obtained because of the difficulty in finely controlling the crystallinity of AIE materials at nanoscale. Herein, we report the preparation of highly luminescent inks via oil‐in‐water microemulsion induced aggregation of Cu–I hybrid clusters based on the highly soluble copper iodide‐tris(3‐methylphenyl)phosphine (Cu4I4(P‐(m‐Tol)3)4) hybrid. Furthermore, we can synthesize a series of AIE inks with different light‐emission colors to cover the whole visible spectrum range via a facile ligand exchange processes. The assemblies of Cu–I hybrid clusters with AIE characteristics will pave the way to fabricate low‐cost highly luminescent inks. [ABSTRACT FROM AUTHOR]

Inorganic perovskite CsPbBr3 nanocrystals (NCs) are emerging, highly attractive light emitters with high color purity and good thermal stability for light-emitting diodes (LEDs). Their high photo/ electroluminescence efficiencies are very important for fabricating efficient LEDs. Here, we propose a novel strategy to enhance the photo/electroluminescence efficiency of CsPbBr3 NCs through doping of heterovalent Ce3+ ions via a facile hot-injection method. The Ce3+ cation was chosen as the dopant for CsPbBr3 NCs by virtue of its similar ion radius and formation of higher energy level of conduction band with bromine in comparison with the Pb2+ cation to maintain the integrity of perovskite structure without introducing additional trap states. It was found that by increasing the doping amount of Ce3+ in CsPbBr3 NCs to 2.88% (atomic percentage of Ce compared to Pb) the photoluminescence quantum yield (PLQY) of CsPbBr3 NCs reached up to 89%, a factor of 2 increase in comparison with the native, undoped ones. The ultrafast transient absorption and time-resolved photoluminescence (PL) spectroscopy revealed that Ce3+-doping can significantly modulate the PL kinetics to enhance the PL efficiency of doped CsPbBr3 NCs. As a result, the LED device fabricated by adopting Ce3+-doped CsPbBr3 NCs as the emitting layers exhibited a pronounced improvement of electroluminescence with external quantum efficiency (EQE) from 1.6 to 4.4% via Ce3+-doping. [ABSTRACT FROM AUTHOR]

Abstract: Low‐dimensional organic–inorganic hybrid perovskites with controllable morphologies are attractive for high‐performance optoelectronic devices. In particular, the 1D organic–inorganic hybrid perovskite nanowires/nanobelts are promising for flexible photodetectors due to high photoresponsivity and strain endurance capability. Herein, a novel and large‐scale synthesis of (C4H9NH3)2PbBr4 organic–inorganic hybrid perovskite nanobelt achieved by the potassium ions assisted controllable crystal growth during the precipitation process in solutions is reported. The obtained (C4H9NH3)2PbBr4 perovskite nanobelts exhibit high‐efficient photoluminescence and superior stability under ambient conditions. Furthermore, these nanobelts are used as photoresponsive materials to fabricate flexible photodetectors, which show much higher switching ratio than that of photodetectors based on (C4H9NH3)2PbBr4 microplatelets. Attractively, after repeated bending for 1000 times, the nanobelt‐based photodetector only shows less than 10% decay in switching ratio in contrast to at least 40% of switching ratio decay for the microplatelets‐based photodetector. The reported potassium ion assisted large‐scale synthesis of (C4H9NH3)2PbBr4 nanobelts paves a new avenue for the application of organic–inorganic hybrid perovskites in flexible optoelectronic devices. [ABSTRACT FROM AUTHOR]

Solution-processable all-inorganic CsPbI 3- x Br x perovskite holds great potential for pure red light-emitting diodes. However, the widely existing defects in this mixed halide perovskite markedly limit the efficiency and stability of present light-emitting diode devices. We here identify that intragrain Ruddlesden-Popper planar defects are primary forms of such defects in the CsPbI 3- x Br x thin film owing to the lattice strain caused by inhomogeneous halogen ion distribution. To eliminate these defects, we develop a stepwise metastable phase crystallization strategy to minimize the CsPbI 3- x Br x perovskite lattice strain, which brings planar defect-free CsPbI 3- x Br x thin film with improved radiative recombination, narrowed emission band, and enhanced spectral stability. Using these high-quality thin films, we fabricate spectrally stable pure red perovskite light-emitting diodes, showing 17.8% external quantum efficiency and 9000 candela meter -2 brightness with color coordinates required by Rec. 2020.

Metal halide perovskites are promising semiconductors for next-generation light-emitting diodes (LEDs) due to their high luminance, excellent color purity, and handily tunable band gap. However, it remains a great challenge to develop perovskite LEDs (PeLEDs) with pure red emission at the wavelength of 630 nm. Herein, we report a spectrally stable and efficient pure red PeLED by employing sequential ligand post-treated CsPbI 3 quantum dots (QDs). The synthesized CsPbI 3 QDs with a size of ∼5 nm are treated in sequential steps using the ligands of 1-hydroxy-3-phenylpropan-2-aminium iodide (HPAI) and tributylsulfonium iodide (TBSI), respectively. The CsPbI 3 QD films exhibit improved optoelectronic properties, which enables the fabrication of a pure red PeLED with a peak external quantum efficiency (EQE) of 6.4% and a stable EL emission centered at the wavelength of 630 nm. Our reported sequential ligand post-treatment strategy opens a new route to improve the stability and efficiency of PeLEDs based on QDs.

Chiral chromophores and their ordered assemblies are intriguing for yielding circularly polarized luminescence (CPL) and exploring intrinsic structure-light emission relationships. With the extensively studied chiral organic molecules and inorganic nanoparticle assemblies for the amplified CPL, the assemblies of copper halide hybrid clusters have attracted intensive attention due to their potential efficient CPL. Here, we report robust chiral phosphine-copper iodide hybrid clusters and their layered assemblies in crystalline states for amplified CPL. We reveal that the intermolecular interactions endow the clusters with the capability of assembling into chiral crystalline CPL materials, including hexagonal platelet-shaped microcrystals ( g lum ≈ 9.5 × 10 -3 ) and highly oriented crystalline films ( g lum ≈ 5 × 10 -3 ). Owing to the high crystalline feature of the thin film, we demonstrate an electroluminescent device with bright electroluminescence (1200 cd m -2 ).

As one fundamental property of light, polarization has a huge impact in quantum optics and optoelectronics through light-matter interactions. However, the bright and near-unity polarized light emissions in the visible range by solid crystalline materials are scantly realized. Here, we report well-defined quasi two-dimensional (2D) hybrid crystals based on the linear alignment of Cu 2 I 2 -dimer/bidentate ligand hybrid clusters for achieving bright and near-unity linearly polarized light emissions. Using first-principle calculations, we demonstrate that the superaligned transition dipole moments are the key for the observed excellent polarized light emissions. To further enhance the photoluminescence (PL) polarization degree, we fabricate Cu 2 I 2 -dimer-based hybrid nanobelts, which display high PL quantum yield (up to 64%) and ultrahigh PL polarization degree (∼0.99). Our reported copper iodine cluster-based luminescent hybrid materials for bright and highly polarized light emissions will have great potential for future quantum optics applications.

Highly luminescent inks are desirable for various applications such as decorative coating, art painting, and anticounterfeiting, to name a few. However, present inks display low photoluminescent efficiency requiring a strong excitation light to make them glow. Here, we report a highly luminescent ink based on the copper-iodide/1-Propyl-1,4-diazabicyclo[2.2.2]octan-1-ium (Cu 4 I 6 (pr-ted) 2 ) hybrid cluster with a quantum efficiency exceeding 98%. Under the interaction between the Cu 4 I 6 (pr-ted) 2 hybrid cluster and polyvinylpyrrolidone (PVP), the highly luminescent Cu 4 I 6 (pr-ted) 2 /PVP ink can be facilely prepared via the one-pot solution synthesis. The obtained ink exhibits strong green light emission that originates from the efficient phosphorescence of Cu 4 I 6 (pr-ted) 2 nanocrystals. Attractively, the ink displays high conversion efficiency for the ultraviolet light to bright green light emission due to its wide Stokes shift, implying great potential for anticounterfeiting and luminescent solar concentrator coating.

All-inorganic lead halide perovskite nanocrystals (NCs) are potential candidates for fabricating high-performance light-emitting diodes (LEDs) owing to their precisely tunable bandgaps, high photoluminescence (PL) efficiency, and excellent color purities. However, the performance of pure red (630-640 nm) all-inorganic perovskite LEDs is still limited by the halide segregation-induced instability of the electroluminescence (EL) of mixed halide CsPbI 3- x Br x NCs. Herein, we report an effective approach to improving the EL stability of pure red all-inorganic CsPbI 3- x Br x NC-based LEDs via the passivation of potassium bromide on NCs. By adding potassium oleate to the reaction system, we obtained potassium bromide surface-passivated (KBr-passivated) CsPbI 3- x Br x NCs with pure red PL emission and a photoluminescence quantum yield (PLQY) exceeding 90%. We determine that most potassium ions present on the surface of NCs bind with bromide ions and thus demonstrate that potassium bromide surface passivation of NCs can both improve the PL stability and inhibit the halide segregation of NCs. Using KBr-passivated CsPbI 3- x Br x NCs as an emitting layer, we fabricated stable and pure red perovskite LEDs with emission at 637 nm, showing a maximum brightness of 2671 cd m -2 , maximum external quantum efficiency of 3.55%, and good EL stability. The proposed KBr-passivated NC strategy will open a new avenue for fabricating efficient, stable, and tunable pure color perovskite NC LEDs.

Cubic phase CsPbI 3 quantum dots (α-CsPbI 3 QDs) as a newly emerging type of semiconducting QDs hold tremendous promise for fundamental research and optoelectronic device applications. However, stable and sub-5 nm-sized α-CsPbI 3 QDs have rarely been demonstrated so far due to their highly labile ionic structure and low phase stability. Here, we report a novel strontium-substitution along with iodide passivation strategy to stabilize the cubic phase of CsPbI 3 , achieving the facile synthesis of α-CsPbI 3 QDs with a series of controllable sizes down to sub-5 nm. We demonstrate that the incorporation of strontium ions can significantly increase the formation energies of α-CsPbI 3 QDs and hence reduce the structure distortion to stabilize the cubic phase at the few-nanometer size. The size ranging from 15 down to sub-5 nm of as-prepared stable α-CsPbI 3 QDs allowed us to investigate their unique size-dependent optical properties. Strikingly, the few-nanometer-sized α-CsPbI 3 QDs turned out to retain high photoluminescence and highly close packing in solid state thin films, and the fabricated red light emitting diodes exhibited high brightness (1250 cd m -2 at 9.2 V) and good operational stability (L 50 > 2 h driven by 6 V). The developed cation-substitution strategy will provide an alternative method to prepare uniform and finely size-controlled colloidal lead halide perovskite QDs for various optoelectronic applications.

Photocoupler is a kind of semiconductor optoelectronic device that integrates light-emitting device (LED) and photodetector. It has found wide application in various fields because of its capability to transmit the electrical signal through the conversion of the electricity-light-electricity. Herein, we report the fabrication of a new photocoupler by simply integrating perovskite quantum dots LED and perovskite photodetector on a glass substrate. The as-fabricated photocoupler showed outstanding characteristics with high current transfer ratio (CTR) of 3.35%, which is highly competitive in comparison with other materials based devices. Furthermore, the perovskite photocoupler had a fast response speed of 8 μs/8.26 μs. By further adding an amplification circuit, the CTR could be enhanced by around 50 times to 172.6%. These results indicate that the present perovskite-based photocouplers may find potential application in future integrated circuit and optoelectronic system.

Although the efficiency of metal halide perovskite light emitting diodes (PeLEDs) has been improved to an attractive level, the poor stability of perovskite emitting layers is a major concern for the application of PeLEDs. Herein, we report a facile ligand-assisted precipitation synthesis of stable dual-phase CsPbBr 3 -CsPb 2 Br 5 nanocrystals (NCs) for improving the stability of PeLEDs. In our synthetic process, the bromide-rich circumstance is beneficial to generate high quality dual-phase perovskite NCs with PLQY as high as 92% and a narrow emission linewidth (19 nm). More importantly, as-synthesized dual phase perovskite NCs exhibit extremely high thermal stability in heating tests in air with a considerable humidity of 30%-55% in comparison with previously reported single phase CsPbBr 3 NCs. The aforementioned advantages of our synthesized dual-phase CsPbBr 3 -CsPb 2 Br 5 NCs allow for the fabrication of light emitting layers of PeLEDs under ambient conditions. The fabricated green PeLED based on CsPbBr 3 -CsPb 2 Br 5 NCs shows a low turn-on voltage of 2.5 V and a high brightness of 8383 cd m -2 at 8 V. Owing to the high stability of dual-phase CsPbBr 3 -CsPb 2 Br 5 NCs, the fabricated PeLED also exhibits better operational stability in comparison with those PeLEDs based on single phase CsPbBr 3 NCs. Our work presents a new route to fabricate stable perovskite light-emitting diodes using room temperature precipitated dual-phase CsPbBr 3 -CsPb 2 Br 5 NCs as emitting layer materials.

Aggregation-induced emission (AIE) is an attractive phenomenon in which materials display strong luminescence in the aggregated solid states rather than in the conventional dissolved molecular states. However, highly luminescent inks based on AIE are hard to be obtained because of the difficulty in finely controlling the crystallinity of AIE materials at nanoscale. Herein, we report the preparation of highly luminescent inks via oil-in-water microemulsion induced aggregation of Cu-I hybrid clusters based on the highly soluble copper iodide-tris(3-methylphenyl)phosphine (Cu 4 I 4 (P-(m-Tol) 3 ) 4 ) hybrid. Furthermore, we can synthesize a series of AIE inks with different light-emission colors to cover the whole visible spectrum range via a facile ligand exchange processes. The assemblies of Cu-I hybrid clusters with AIE characteristics will pave the way to fabricate low-cost highly luminescent inks., (© 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Inorganic perovskite CsPbBr 3 nanocrystals (NCs) are emerging, highly attractive light emitters with high color purity and good thermal stability for light-emitting diodes (LEDs). Their high photo/electroluminescence efficiencies are very important for fabricating efficient LEDs. Here, we propose a novel strategy to enhance the photo/electroluminescence efficiency of CsPbBr 3 NCs through doping of heterovalent Ce 3+ ions via a facile hot-injection method. The Ce 3+ cation was chosen as the dopant for CsPbBr 3 NCs by virtue of its similar ion radius and formation of higher energy level of conduction band with bromine in comparison with the Pb 2+ cation to maintain the integrity of perovskite structure without introducing additional trap states. It was found that by increasing the doping amount of Ce 3+ in CsPbBr 3 NCs to 2.88% (atomic percentage of Ce compared to Pb) the photoluminescence quantum yield (PLQY) of CsPbBr 3 NCs reached up to 89%, a factor of 2 increase in comparison with the native, undoped ones. The ultrafast transient absorption and time-resolved photoluminescence (PL) spectroscopy revealed that Ce 3+ -doping can significantly modulate the PL kinetics to enhance the PL efficiency of doped CsPbBr 3 NCs. As a result, the LED device fabricated by adopting Ce 3+ -doped CsPbBr 3 NCs as the emitting layers exhibited a pronounced improvement of electroluminescence with external quantum efficiency (EQE) from 1.6 to 4.4% via Ce 3+ -doping.