Metal-halide perovskites have rapidly emerged as one of the most promising materials of the 21st century, with many exciting properties and great potential for a broad range of applications, from photovoltaics to optoelectronics and photocatalysis. The ease with which metal-halide perovskites can be synthesized in the form of brightly luminescent colloidal nanocrystals, as well as their tunable and intriguing optical and electronic properties, has attracted researchers from different disciplines of science and technology. In the last few years, there has been a significant progress in the shape-controlled synthesis of perovskite nanocrystals and understanding of their properties and applications. In this comprehensive review, researchers having expertise in different fields (chemistry, physics, and device engineering) of metal-halide perovskite nanocrystals have joined together to provide a state of the art overview and future prospects of metal-halide perovskite nanocrystal research.
While perovskite nanocrystals (NCs) have shown great promise as materials for efficient light-emitting diodes (LEDs), low photoluminescence quantum yield (PLQY) of the blue-emitting perovskites is an impediment to the development of white LEDs of which blue is an essential component. Herein, we report that room temperature postsynthetic treatment of weakly blue-violet-emitting (PLQY 3%) CsPbCl3 NCs with CdCl2 results in an instantaneous enhancement of the PLQY to near-unity without affecting the PL peak position (406 nm) and spectral width. The time-resolved PL and ultrafast transient absorption measurements confirm the removal of nonradiative defect states of the CsPbCl3 NCs in treated sample. The elemental composition and structural data of the treated sample reveal facile doping of Cd2+ into the crystal lattice without affecting the size and shape of the NCs. Extraordinary PLQY, high air stability and photostability and ease of preparation of this Cd-doped CsPbCl3 make it by far the most attractive blue-emitting perovskite for development of efficient blue and white LEDs.
Mn-Doped perovskite nanocrystals (NCs) are a new class of materials offering exciting opportunities to control over their optical and magnetic properties. Herein, we report a series of Mn-doped CsPbCl NCs exhibiting a tunable Mn photoluminescence (PL) band with a PL peak wavelength pushed up to 625 nm and tuned over a range of 40 nm, the largest achieved so far, by only varying the Mn content. The X-band EPR data and Mn PL decay behaviour of the NCs reveal that the exchange interaction between Mn ions is mainly responsible for a large shift of the Mn PL band. Ultrafast pump-probe measurements show that exciton-dopant energy transfer in these NCs is slower (∼50-100 ps) than trapping of the carriers (∼8-10 ps) in the host lattice. The large PL tuning reported here along with the insights into the mechanism of tuning and carrier dynamics are expected to boost the potential of Mn-doped CsPbCl NCs in light-powered devices.
Defects have always been an integral part of semiconductor crystals, controlling their optical and electronic properties. Even though growing popularity of the CsPbX 3 (X = Cl, Br, I, and their mixture) nanocrystals (NCs) in various applications stems from their defect-tolerant nature, the properties, stability, and practical utility of these substances are still very much governed by the defects. A variety of methods, which are halide-specific, have been developed to regulate the activities of the defects for enhancing the photoluminescence and stability of these NCs. In this Perspective, we trace the origin and manifestation of different types of defects in photoluminescence properties and stability of the CsPbX 3 NCs, critically examine the rationale of various passivation strategies to obtain an in-depth understanding of the problem, and recommend the most effective strategy to be followed for tackling defects under any given condition.
The lack of long-term stability, the presence of toxic lead, and a low photoluminescence (PL) efficiency are the major obstacles to the commercialization of lead-halide perovskite-based optoelectronic and photovoltaic devices. Herein we report a facile ambient condition doping protocol that addresses all three issues of the CsPbX 3 perovskite nanocrystals (NCs) to a substantial extent. We show that the roomtemperature treatment of these NCs with MgX 2 results in the partial (18−23%) replacement of toxic lead, enhances the PL quantum yield of green-emitting CsPbBr 3 (to ∼100% from ∼51%) and violet-emitting CsPbCl 3 NCs (to ∼79% from ∼1%), and improves the stability under ambient conditions and in the presence of light and a polar solvent. Ultrafast pump−probe and temperature-dependent PL studies reveal that curing of the intrinsic structural disorder, introduction of some shallow energy levels close to the conduction band edge, and effective passivation of the halide deficiency contribute to the improved properties of the doped systems.
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