Changing the Dimensionality of Cesium Lead Bromide Nanocrystals by Reversible Postsynthesis Transformations with Amines

Palazón, Francisco; Almeida, Guilherme; Akkerman, Quinten A.; Trizio, Luca De; Dang, Zhiya; Prato, Mirko; Manna, Liberato

doi:10.1021/acs.chemmater.7b00895

Cited by 148 publications

(201 citation statements)

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“…The versatility of the Cs–Pb–X ternary compounds (particularly Cs 4 PbX 6 and CsPbX 3 ) lies in their ability to interconversion via post-synthetic physical and chemical treatments 29 . The post-synthetic conversion of cubic CsPbX 3 to rhombohedral Cs 4 PbX 6 has been demonstrated via amine- and thiol-mediated extraction of PbBr 2 30 , while the reverse conversion from Cs 4 PbX 6 to CsPbX 3 has been reported by the insertion of PbX 2 , stripping of CsX, excess oleic acid, and by heat treatment (90 to 180 °C) 18 .…”

Section: Resultsmentioning

confidence: 99%

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Probing molecule-like isolated octahedra via phase stabilization of zero-dimensional cesium lead halide nanocrystals

et al. 2018

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Zero-dimensional (0D) inorganic perovskites have recently emerged as an interesting class of material owing to their intrinsic Pb2+ emission, polaron formation, and large exciton binding energy. They have a unique quantum-confined structure, originating from the complete isolation of octahedra exhibiting single-molecule behavior. Herein, we probe the optical behavior of single-molecule-like isolated octahedra in 0D Cesium lead halide (Cs4PbX6, X = Cl, Br/Cl, Br) nanocrystals through isovalent manganese doping at lead sites. The incorporation of manganese induced phase stabilization of 0D Cs4PbX6 over CsPbX3 by lowering the symmetry of PbX6 via enhanced octahedral distortion. This approach enables the synthesis of CsPbX3 free Cs4PbX6 nanocrystals. A high photoluminescence quantum yield for manganese emission was obtained in colloidal (29%) and solid (21%, powder) forms. These performances can be attributed to structure-induced confinement effects, which enhance the energy transfer from localized host exciton states to Mn2+ dopant within the isolated octahedra.

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Section: Resultsmentioning

confidence: 99%

“…CsPbX 3 (X = Br, Br/Cl, Cl) nanocrystals were synthesized as described by Palazon et al 29 . In a typical synthesis, PbX 2 (0.2 mmol; X = Br, Cl, Br/Cl), 0.47 mL oleic acid, 5.0 mL octadecene, and 0.50 mL oleylamine were loaded in a 25 mL 3-neck flask and dried under vacuum at 100 °C for 15 min.…”

Section: Methodsmentioning

confidence: 99%

Probing molecule-like isolated octahedra via phase stabilization of zero-dimensional cesium lead halide nanocrystals

et al. 2018

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“…Based on the rhombohedral shapes observed by transmission electron microscopy (TEM) and more importantly on the XRD signal especially at long milling times, we infer that Cs 4 PbBr 6 is formed under certain conditions. This is plausible, as it is known that oleylamine can induce the transformation of preformed CsPbBr 3 into Cs 4 PbBr 6 . Nevertheless, this highlights an important point for the two‐step approach of making perovskite QDs, which is that addition of ligands (necessary for colloidal stability) may also result in unwanted further chemical reactions.…”

Section: Mcs For the Production Of High‐purity Lhpsmentioning

confidence: 99%

Making by Grinding: Mechanochemistry Boosts the Development of Halide Perovskites and Other Multinary Metal Halides

Palazón

Ajjouri

Bolink

2019

Advanced Energy Materials

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101

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Mechanochemical synthesis has recently emerged as a promising route for the synthesis of functional lead halide perovskites as well as other (lead‐free) metal halides. Mechanochemical synthesis presents several advantages with regards to more commonly used solution‐based processes such as an inherent lower toxicity by avoiding organic solvents and a finer control over stoichiometry of the final products. The ease of implementation, either through the use of a simple mortar and pestle or with an electrically powered ball‐mill, and low amount of side products make mechanochemical synthesis appealing for upscaling the production of halide perovskites. Due to the defect tolerance of lead halide perovskites, they are ideally suited to be prepared by this solvent‐free method. However, the implementation of these semiconductors in high‐efficiency optoelectronic devices requires the transformation of synthesized powder into smooth thin films where still some hurdles remain to be cleared.

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“…Recently, we have shown in our group that direct lithography on QD films either with electron beams or Xrays leads not only to an enhanced adhesion to the substrate but also makes the exposed regions less prone to undergo various chemical transformations, as they become partially sealed off from the external environment. (113)(114)(115) For instance, we demonstrated that pristine TOPO-capped CdSe/CdS NC films can be transformed to Cu2Se/Cu2S by cation-exchange reactions with copper precursors. Note that, in this case, these precursors were dissolved in solvents in which the NCs themselves were not dispersible, otherwise the film would have been damaged.…”

Section: Beyond Simple Patterning: Tuning Ncs' Chemical Reactivitymentioning

confidence: 99%

Writing on Nanocrystals: Patterning Colloidal Inorganic Nanocrystal Films through Irradiation-Induced Chemical Transformations of Surface Ligands

2017

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In the past couple of decades, colloidal inorganic nanocrystals (NCs) and, more specifically, semiconductor quantum dots (QDs) have emerged as crucial materials for the development of nanoscience and nanotechnology, with applications in very diverse areas such as optoelectronics and biotechnology. Films made of inorganic NCs deposited on a substrate can be patterned by e-beam lithography, altering the structure of their capping ligands and thus allowing exposed areas to remain on the substrate while non-exposed areas are redispersed in a solvent, as in a standard lift-off process. This methodology can be described as a “direct” lithography process, since the exposure is performed directly on the material of interest, in contrast with conventional lithography which uses a polymeric resist as a mask for subsequent material deposition (or etching). A few reports from the late 1990s and early 2000s used such direct lithography to fabricate electrical wires from metallic NCs. However, the poor conductivity obtained through this process hindered the widespread use of the technique. In the early 2010s, the same method was used to define fluorescent patterns on QD films, allowing for further applications in biosensing. For the past 2–3 years, direct lithography on NC films with e-beams and X-rays has gone through an important development as it has been demonstrated that it can tune further transformations on the NCs, leading to more complex patternings and opening a whole new set of possible applications. This Perspective summarizes the findings of the past 20 years on direct lithography on NC films with a focus on the latest developments on QDs from 2014 and provides different potential future outcomes of this promising technique.

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Changing the Dimensionality of Cesium Lead Bromide Nanocrystals by Reversible Postsynthesis Transformations with Amines

Cited by 148 publications

References 33 publications

Probing molecule-like isolated octahedra via phase stabilization of zero-dimensional cesium lead halide nanocrystals

Probing molecule-like isolated octahedra via phase stabilization of zero-dimensional cesium lead halide nanocrystals

Making by Grinding: Mechanochemistry Boosts the Development of Halide Perovskites and Other Multinary Metal Halides

Writing on Nanocrystals: Patterning Colloidal Inorganic Nanocrystal Films through Irradiation-Induced Chemical Transformations of Surface Ligands

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