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Colloidal Aziridinium Lead Bromide Quantum Dots.

ABSTRACT: The compositional engineering of lead-halide perovskite nanocrystals (NCs) via the A-site cation represents a lever to fine-tune their structural and electronic properties. However, the presently available chemical space remains minimal since, thus far, only three A-site cations have been reported to favor the formation of stable lead-halide perovskite NCs, i.e., Cs⁺, formamidinium (FA), and methylammonium (MA). Inspired by recent reports on bulk single crystals with aziridinium (AZ) as the A-site cation, we present a facile colloidal synthesis of AZPbBr₃ NCs with a narrow size distribution and size tunability down to 4 nm, producing quantum dots (QDs) in the regime of strong quantum confinement. NMR and Raman spectroscopies confirm the stabilization of the AZ cations in the locally distorted cubic structure. AZPbBr₃ QDs exhibit bright photoluminescence with quantum efficiencies of up to 80%. Stabilized with cationic and zwitterionic capping ligands, single AZPbBr₃ QDs exhibit stable single-photon emission, which is another essential attribute of QDs. In particular, didodecyldimethylammonium bromide and 2-octyldodecyl-phosphoethanolamine ligands afford AZPbBr₃ QDs with high spectral stability at both room and cryogenic temperatures, reduced blinking with a characteristic ON fraction larger than 85%, and high single-photon purity (g⁽²⁾(0) = 0.1), all comparable to the best-reported values for MAPbBr₃ and FAPbBr₃ QDs of the same size.

SUBMITTER: Bodnarchuk MI

PROVIDER: S-EPMC10883123 | biostudies-literature | 2024 Feb

REPOSITORIES: biostudies-literature

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Colloidal Aziridinium Lead Bromide Quantum Dots.

Bodnarchuk Maryna I MI Feld Leon G LG Zhu Chenglian C Boehme Simon C SC Bertolotti Federica F Avaro Jonathan J Aebli Marcel M Mir Showkat Hassan SH Masciocchi Norberto N Erni Rolf R Chakraborty Sudip S Guagliardi Antonietta A Rainò Gabriele G Kovalenko Maksym V MV

ACS nano 20240206

The compositional engineering of lead-halide perovskite nanocrystals (NCs) via the A-site cation represents a lever to fine-tune their structural and electronic properties. However, the presently available chemical space remains minimal since, thus far, only three A-site cations have been reported to favor the formation of stable lead-halide perovskite NCs, i.e., Cs<sup>+</sup>, formamidinium (FA), and methylammonium (MA). Inspired by recent reports on bulk single crystals with aziridinium (AZ) ...[more]

PMID: 38320982

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Project description:Pairs of coupled quantum dots with controlled coupling between the two potential wells serve as an extremely rich system, exhibiting a plethora of optical phenomena that do not exist in each of the isolated constituent dots. Over the past decade, coupled quantum systems have been under extensive study in the context of epitaxially grown quantum dots (QDs), but only a handful of examples have been reported with colloidal QDs. This is mostly due to the difficulties in controllably growing nanoparticles that encapsulate within them two dots separated by an energetic barrier via colloidal synthesis methods. Recent advances in colloidal synthesis methods have enabled the first clear demonstrations of colloidal double quantum dots and allowed for the first exploratory studies into their optical properties. Nevertheless, colloidal double QDs can offer an extended level of structural manipulation that allows not only for a broader range of materials to be used as compared with epitaxially grown counterparts but also for more complex control over the coupling mechanisms and coupling strength between two spatially separated quantum dots. The photophysics of these nanostructures is governed by the balance between two coupling mechanisms. The first is via dipole-dipole interactions between the two constituent components, leading to energy transfer between them. The second is associated with overlap of excited carrier wave functions, leading to charge transfer and multicarrier interactions between the two components. The magnitude of the coupling between the two subcomponents is determined by the detailed potential landscape within the nanocrystals (NCs). One of the hallmarks of double QDs is the observation of dual-color emission from a single nanoparticle, which allows for detailed spectroscopy of their properties down to the single particle level. Furthermore, rational design of the two coupled subsystems enables one to tune the emission statistics from single photon emission to classical emission. Dual emission also provides these NCs with more advanced functionalities than the isolated components. The ability to better tailor the emission spectrum can be advantageous for color designed LEDs in lighting and display applications. The different response of the two emission colors to external stimuli enables ratiometric sensing. Control over hot carrier dynamics within such structures allows for photoluminescence upconversion. This Account first provides a description of the main hurdles toward the synthesis of colloidal double QDs and an overview of the growing library of synthetic pathways toward constructing them. The main discoveries regarding their photophysical properties are then described in detail, followed by an overview of potential applications taking advantage of the double-dot structure. Finally, a perspective and outlook for their future development is provided.

Dataset Information

Colloidal Aziridinium Lead Bromide Quantum Dots.

Publications

Colloidal Aziridinium Lead Bromide Quantum Dots.

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