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Role of Acid-Base Equilibria in the Size, Shape, and Phase Control of Cesium Lead Bromide Nanocrystals.

ABSTRACT: A binary ligand system composed of aliphatic carboxylic acids and primary amines of various chain lengths is commonly employed in diverse synthesis methods for CsPbBr3 nanocrystals (NCs). In this work, we have carried out a systematic study examining how the concentration of ligands (oleylamine and oleic acid) and the resulting acidity (or basicity) affects the hot-injection synthesis of CsPbBr3 NCs. We devise a general synthesis scheme for cesium lead bromide NCs which allows control over size, size distribution, shape, and phase (CsPbBr3 or Cs4PbBr6) by combining key insights on the acid-base interactions that rule this ligand system. Furthermore, our findings shed light upon the solubility of PbBr2 in this binary ligand system, and plausible mechanisms are suggested in order to understand the ligand-mediated phase control and structural stability of CsPbBr3 NCs.

SUBMITTER: Almeida G

PROVIDER: S-EPMC5830690 | biostudies-literature | 2018 Feb

REPOSITORIES: biostudies-literature

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Role of Acid-Base Equilibria in the Size, Shape, and Phase Control of Cesium Lead Bromide Nanocrystals.

Almeida Guilherme G Goldoni Luca L Akkerman Quinten Q Dang Zhiya Z Khan Ali Hossain AH Marras Sergio S Moreels Iwan I Manna Liberato L

ACS nano 20180213 2

A binary ligand system composed of aliphatic carboxylic acids and primary amines of various chain lengths is commonly employed in diverse synthesis methods for CsPbBr<sub>3</sub> nanocrystals (NCs). In this work, we have carried out a systematic study examining how the concentration of ligands (oleylamine and oleic acid) and the resulting acidity (or basicity) affects the hot-injection synthesis of CsPbBr<sub>3</sub> NCs. We devise a general synthesis scheme for cesium lead bromide NCs which all ...[more]

PMID: 29381326

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Project description:Metal halide perovskite nanocrystals, an emerging class of materials for advanced photonic and optoelectronic applications, are mainly fabricated with colloidal chemistry routes. On the quest for new properties according to application needs, new perovskite systems of various morphologies and levels of doping and alloying have been developed, often also involving post-synthesis reactions. Recently, laser irradiation in liquids has been utilized as a fast method to synthesize or transform materials and interesting laser-induced transformations on nanocrystals were induced. These studies in general have been limited to small nanocrystals (~15 nm). In the case of halide perovskites, fragmentation or anion exchange have been observed in such laser-based processes, but no crystal structure transformations were actually observed or deliberately studied. Nanocrystals are more sensitive to light exposure compared to the corresponding bulk crystals. Additional factors, such as size, morphology, the presence of impurities, and others, can intricately affect the photon absorption and heat dissipation in nanocrystal suspensions during laser irradiation. All these factors can play an important role in the final morphologies and in the time required for these transformations to unfold. In the present work, we have employed a 513 nm femtosecond (fs) laser to induce different transformations in large nanocrystals, in which two phases coexist in the same particle (Cs4PbBr6/CsPbBr3 nanohexagons of ~100 nm), dispersed in dichlorobenzene. These transformations include: (i) the exfoliation of the primary nanohexagons and partial anion exchange; (ii) fragmentation in smaller nanocubes and partial anion exchange; (iii) side-by-side-oriented attachment, fusion, and formation of nanoplatelets and complete anion exchange; (iv) side-by-side attachment, fusion, and formation of nanosheets. Partial or complete Br-Cl anion exchange in the above transformations was triggered by the partial degradation of dichlorobenzene. In addition to the detailed analysis of the various nanocrystal morphologies observed in the various transformations, the structure-photoluminescence relationships for the different samples were analyzed and discussed.

Dataset Information

Role of Acid-Base Equilibria in the Size, Shape, and Phase Control of Cesium Lead Bromide Nanocrystals.

Publications

Role of Acid-Base Equilibria in the Size, Shape, and Phase Control of Cesium Lead Bromide Nanocrystals.

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