In this work we study the kinetics of cesium lead halide perovskite nanoparticle (NP) growth; the focusing and de-focusing of the NP size distribution. Cesium lead halide perovskite NPs are considered to be attractive materials for optoelectronic applications. Understanding the kinetics of the formation of these all-inorganic perovskite NPs is critical for reproducibly and reliably generating large amounts of uniformly sized NPs. Here we investigate different growth durations for CsPbI3 and CsPbBr3 NPs, tracking their growth by high-resolution transmission electron microscopy and size distribution analysis. As a result, we are able to provide a detailed model for the kinetics of their growth. It was observed that the CsPbI3 NPs exhibit focusing of the size distribution in the first 20 seconds of growth, followed by de-focusing over longer growth durations, while the CsPbBr3 NPs show de-focusing of the size distribution starting from the beginning of the growth. The monomer concentration is depleted faster in the case of CsPbBr3 than in the case of CsPbI3, due to faster diffusion of the monomers, which increases the critical radius and results in de-focusing of the population. Accordingly, focusing is not observed within 40 seconds of growth in the case of CsPbBr3. This study provides important knowledge on how to achieve a narrow size distribution of cesium lead halide perovskite NPs when generating large amounts of these promising, highly luminescent NPs.
Perovskite nanostructures, both hybrid organo-metal and fully inorganic perovskites, have gained a lot of interest in the past few years for their intriguing optical properties in the visible region. We report on inorganic cesium lead bromide (CsPbBr) nanowires (NWs) having quantum confined dimensions corresponding to 5 unit cells. The addition of various hydrohalic acids (HX, X = Cl, Br, I) was found to highly affect the NW length, composition, and optical properties. Hydrochloric (HCl) and hydroiodic (HI) acids mixed in the reaction solution influence the crystal structure and optical properties and shorten the NWs, while the hydrobromic acid (HBr) addition results solely in shorter NWs, without any structural change. The addition of HX increases the acidity of the reaction solution, resulting in protonation of the oleylamine ligands from oleylamine into oleyl-ammonium cations that behave similarly to Cs during crystallization. Therefore, the positions of the Cs at the growing surface of the NWs are taken by the oleyl-ammonium cations, thus blocking further growth in the favored direction. The emission of the NWs is tunable between ∼423-505 nm and possesses a potential in the optoelectronic field. Moreover, electrical conductivity measurements of the NWs are discussed to give a new point of view regarding the conductivity of perovskite nanostructures.
One of the most attractive features of perovskite materials is their chemical flexibility. Due to innovative chemical compositions of perovskites, their optical and structural properties, and functionalities have become more advanced, enabling better solar performance in photovoltaics, as well as robustness and excellent properties in the nanoscale for optoelectronics. The quest for novel perovskite compositions in the nano-scale is significantly important. This paper reports on a mixed-cation system of RbxCs1-xPbX3 (where X = Cl or Br) nanoparticles. The absorption of the nanoparticles is tunable in the near ultra-violet and visible regions between ∼395-525 nm for RbxCs1-xPbX3 (x = 0 to x = 0.8 and X = Cl or Br). The photoluminescence quantum yields (PLQY) of the mixed Rb+/Cs+ nanoparticle systems are comparable to the PLQY of CsPbX3 nanoparticles. Interestingly an attempt to synthesize Cl- and Br-based nanoparticles with high Rb+ content was successful, although possessing low tolerance factors. We conclude that these mixed Rb+/Cs+ nanoparticles are more adjustable to structural distortions caused by cation substitutions than their bulk counterparts, which opens a way towards the development of more advanced mixed-ion perovskite compositions in the nano-scale.
Hybrid perovskite and all‐inorganic perovskite have attracted much attention in recent years owing to their successful use in the photovoltaic field. Usually the perovskite is used in its bulk form, although recently, perovskites' nanocrystalline form has received increased attention. Recent developments in the evolving research field of nanomaterial‐based perovskite are reviewed. Both hybrid organic‐inorganic and all‐inorganic perovskite nanostructures are discussed, as well as approaches to tune the optical properties by controlling the size and shape of perovskite nanostructures. In addition, chemical modifications can change the perovskite nanostructures' band‐gap, similar to their bulk counterpart. Several applications, including light‐emitting diodes, lasers, and detectors, demonstrate the latent potential of perovskite nanostructures.
Excitons in colloidal semiconductor nanoplatelets (NPLs) are weakly confined in the lateral dimensions. This results in significantly smaller Auger rates and, consequently, larger biexciton quantum yields, when compared to spherical quantum dots (QDs). Here we report a study of the temperature dependence of the biexciton Auger rate in individual CdSe/CdS core–shell NPLs, through the measurement of time-gated second-order photon correlations in the photoluminescence. We also utilize this method to directly estimate the single-exciton radiative rate. We find that whereas the radiative lifetime of NPLs increases with temperature, the Auger lifetime is almost temperature-independent. Our findings suggest that Auger recombination in NPLs is qualitatively similar to that of semiconductor quantum wells. Time-gated photon correlation measurements offer the unique ability to study multiphoton emission events, while excluding effects of competing fast processes, and can provide significant insight into the photophysics of a variety of nanocrystal multiphoton emitters.
Colloidal semiconductor nanoplatelets, in which carriers are strongly confined only along one dimension, present fundamentally different excitonic properties than quantum dots, which support strong confinement in all three dimensions. In particular, multiple excitons strongly confined in just one dimension are free to re-arrange in the lateral plane, reducing the probability for multi-body collisions. Thus, while simultaneous multiple photon emission is typically quenched in quantum dots, in nanoplatelets its probability can be tuned according to size and shape. Here, we focus on analyzing multi-exciton dynamics in individual CdSe/CdS nanoplatelets of various sizes through the measurement of second-, third-, and fourth-order photon correlations. Thus, for the first time, we can directly probe the dynamics of the two, three and four exciton states in the single nanocrystal level. Remarkably, although higher orders of correlation vary substantially among the synthesis' products, they strongly correlate with the value of second order antibunching. The scaling of the higher order moments with the degree of antibunching presents a small yet clear deviation from the accepted model of Auger recombination through binary collisions. Such a deviation suggests that many-body contributions are present already at the level of triexcitons. These findings highlight the benefit of high-order photon correlation spectroscopy as a technique to study multi-exciton dynamics in colloidal semiconductor nanocrystals.
Alkali ternary lead halides were studied intensively in the past few years, especially due to the great interest in perovskite materials. In this paper we report on novel rubidium lead chloride nanocrystals (NCs) with the formula Rb 6 Pb 5 Cl 16 , which adopt a tetragonal symmetry. The NCs were characterized and found to be active in the UV region, with a band-gap of ~4.05 eV. The roles of the ligands, oleic acid and oleylamine, were investigated and found to strongly affect the morphology and composition of the NCs, through the stabilization of the facilitated crystallization of the ionic precursors. The effective masses were observed by density functional theory (DFT) calculations, using the dielectric function, and the the Bohr exciton radius and exciton binding energy of the NCs were estimated. Morover the results were supported by the DFT calculations for the electronic properties and atomic structure.
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