Size-tunable and stable cesium lead-bromide perovskite nanocubes with near-unity photoluminescence quantum yield

Grisorio, Roberto; Conelli, Daniele; Fanizza, Elisabetta; Striccoli, Marinella; Altamura, Davide; Giannini, Cinzia; Allegretta, Ignazio; Terzano, Roberto; Irimia‐Vladu, Mihai; Margiotta, Nicola; Suranna, Gian Paolo

doi:10.1039/d1na00142f

Cited by 12 publications

(10 citation statements)

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“…32 The dispersion of the chosen lead precursor (PbBr 2 ) in toluene was accomplished by the presence of an equimolar amount of (n-Hept) 4 NBr salt, promoting the formation of soluble intermediates. 33 The modulation of the halide component (to regard the blue region in emission for the corresponding NCs, vide inf ra) was subsequently performed by introducing the suitable quantity of dimethyldioctadecylammonium chloride (DODC) in the reaction mixture (PbBr 2 /DODC = 5:1 mol/mol) before the cesium injection, as schematized in Figure 1. Notwithstanding the structural analogy of the two organic cations used in this synthetic sequence, we observed that the presence of (n-Hept) 4 NBr in the first step was indispensable for warranting the complete dissolution of the lead precursor, which does not occur by utilizing only DODC as a surfactant even at higher concentrations.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

“…This route allowed to bypass the conventional dissolution step of the ionic precursors of LHP NCs requiring high temperatures or aggressive polar solvents . The dispersion of the chosen lead precursor (PbBr 2 ) in toluene was accomplished by the presence of an equimolar amount of ( n -Hept) 4 NBr salt, promoting the formation of soluble intermediates . The modulation of the halide component (to regard the blue region in emission for the corresponding NCs, vide infra ) was subsequently performed by introducing the suitable quantity of dimethyldioctadecylammonium chloride (DODC) in the reaction mixture (PbBr 2 /DODC = 5:1 mol/mol) before the cesium injection, as schematized in Figure .…”

Section: Results and Discussionmentioning

confidence: 99%

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Synthetic Control over the Surface Chemistry of Blue-Emitting Perovskite Nanocrystals for Photocatalysis

Grisorio

Dibenedetto

Matuhina

et al. 2023

ACS Appl. Nano Mater.

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Lead halide perovskite nanocrystals (NCs) are particularly suitable for light-emitting and photocatalysis applications, where their potential can be maximized by controlling the surface composition of their organic shell. In this study, the preparation of CsPbCl x Br 3−x NCs at room temperature in toluene is described. Three differently structured surfactants are utilized for the synthesis, each with a specific function, namely, the solubilization of the lead precursor (n-Hept 4 NBr), the surface passivation with halide modification (dimethyldioctadecylammonium chloride), and the protection of the surface-active sites (octanoic acid) for photocatalysis. Under these conditions, nearly monodispersed blueemitting nanocubes are selectively obtained in a one-pot synthesis by combining specific amounts of the perovskite precursors. As supported by thermogravimetric analysis (TGA) and Fourier transform infrared (FT-IR) spectroscopy investigations, the organic shell of the obtained NCs is composed of electrostatically bound dimethyldioctadecylammonium ions, granting robustness to the corresponding NCs, and octanoic acid molecules, interacting with the nanoparticle surface through weaker secondary bonds. The obtained NCs exhibit a high photoluminescence quantum yield (PLQY = 72 ± 3%) notwithstanding multiexponential recombination dynamics of the excited state, resulting from the different passivation modes at the NC surface. Moreover, the NCs show a remarkable optical stability after exposure to high temperatures and to water contact due to the high surface density of the multifunctional organic ligands. The introduction of 4-tert-butylphenyl thiol promotes a charge transfer process at the NC/thiol interface formed upon removal of the labile ligands (octanoic acid) at the NC surface. In these conditions, the NCs are prone to the photoinduced conversion of the aromatic thiol into the corresponding disulfide without varying the optical properties of the perovskite photocatalyst upon the substrate conversion. Therefore, the obtained results cast light on the versatility of the surface engineering of lead halide perovskite NCs for efficient blue emission and photocatalysis with improved stability.

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Section: ■ Results and Discussionmentioning

confidence: 99%

Section: Results and Discussionmentioning

confidence: 99%

Synthetic Control over the Surface Chemistry of Blue-Emitting Perovskite Nanocrystals for Photocatalysis

Grisorio

Dibenedetto

Matuhina

et al. 2023

ACS Appl. Nano Mater.

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“…Our results of quantum-confined blue emission from perovskite NCs provide an alternative to mixed halide perovskites and, together with its enhanced stability, could be useful in the realization of blue perovskite LEDs. The PLQY for the green emitting NCs is also high, though rather comparable to other synthesis method [39][40][41]. Yet, the advantage of the mechanochemical synthesis method is the high material yield, providing grams of NCs in a one-pot synthesis in just 1 h.…”

Section: Resultsmentioning

confidence: 72%

Mechanochemical synthesis of stable, quantum-confined CsPbBr₃ perovskite nanocrystals with blue-green emission and high PLQY

et al. 2022

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Cesium lead halides are a family of bright, visible-light emitting materials with near-unity photoluminescence quantum yield (PLQY) in nanocrystals (NCs). The usual way to achieve visible light-emission tunability is by mixing halides, which often leads to phase separation and poor stability. While the NCs should also show size-dependent PL emission, reports on strong quantum confinement in these materials are scarce. Here, we report the synthesis of quantum-confined cesium lead bromide (CsPbBr3) NCs via a facile, environment-friendly, and scalable high-energy mechanochemical synthesis route. The PLQY measured is ~85 %, even after 90 days of synthesis, and the emission wavelength is shifted from green, 520nm, to blue, 460nm by quantum confinement in NCs of size 3-5 nm. Micro-PL optical spectroscopy and atomic force microscopy confirm the size tunability of PL on a single-dot scale. Our work demonstrates the potential of mechanochemical synthesis in the medium-scale production of bright luminescent quantum-confined NCs that could be extended to other materials as well.

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“…Despite significant progress in the thickness‐controlled synthesis with monolayer precision, pristine perovskite NPls usually suffer from low PLQY and colloidal instability as compared with nanocubes. [ 9,14,72,105 ] Although near‐unity PLQY is easily achievable for perovskite nanocubes under optimized conditions, [ 118–120 ] it has been often observed that the PL efficiency decreases for NPLs with decreasing thickness and therefore wide bandgaps. [ 28,29,71 ] In principle, 2D NPls are expected to exhibit high PLQY due to the enhanced radiative recombination caused by the confinement of charge carriers.…”

Section: Synthesis Of Nanoplateletsmentioning

confidence: 99%

Colloidal Metal‐Halide Perovskite Nanoplatelets: Thickness‐Controlled Synthesis, Properties, and Application in Light‐Emitting Diodes

et al. 2022

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Colloidal metal‐halide perovskite nanocrystals (MHP NCs) are gaining significant attention for a wide range of optoelectronics applications owing to their exciting properties, such as defect tolerance, near‐unity photoluminescence quantum yield, and tunable emission across the entire visible wavelength range. Although the optical properties of MHP NCs are easily tunable through their halide composition, they suffer from light‐induced halide phase segregation that limits their use in devices. However, MHPs can be synthesized in the form of colloidal nanoplatelets (NPls) with monolayer (ML)‐level thickness control, exhibiting strong quantum confinement effects, and thus enabling tunable emission across the entire visible wavelength range by controlling the thickness of bromide or iodide‐based lead‐halide perovskite NPls. In addition, the NPls exhibit narrow emission peaks, have high exciton binding energies, and a higher fraction of radiative recombination compared to their bulk counterparts, making them ideal candidates for applications in light‐emitting diodes (LEDs). This review discusses the state‐of‐the‐art in colloidal MHP NPls: synthetic routes, thickness‐controlled synthesis of both organic–inorganic hybrid and all‐inorganic MHP NPls, their linear and nonlinear optical properties (including charge‐carrier dynamics), and their performance in LEDs. Furthermore, the challenges associated with their thickness‐controlled synthesis, environmental and thermal stability, and their application in making efficient LEDs are discussed.

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Size-tunable and stable cesium lead-bromide perovskite nanocubes with near-unity photoluminescence quantum yield

Abstract: Stable cesium lead bromide perovskite nanocrystals (NCs) showing near-unity photoluminescence quantum yield (PLQY), narrow emission profile, and tunable fluorescence peak in the green region can be considered the ideal class...

Cited by 12 publications

References 59 publications

Synthetic Control over the Surface Chemistry of Blue-Emitting Perovskite Nanocrystals for Photocatalysis

Synthetic Control over the Surface Chemistry of Blue-Emitting Perovskite Nanocrystals for Photocatalysis

Mechanochemical synthesis of stable, quantum-confined CsPbBr₃ perovskite nanocrystals with blue-green emission and high PLQY

Colloidal Metal‐Halide Perovskite Nanoplatelets: Thickness‐Controlled Synthesis, Properties, and Application in Light‐Emitting Diodes

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Size-tunable and stable cesium lead-bromide perovskite nanocubes with near-unity photoluminescence quantum yield

Abstract: Stable cesium lead bromide perovskite nanocrystals (NCs) showing near-unity photoluminescence quantum yield (PLQY), narrow emission profile, and tunable fluorescence peak in the green region can be considered the ideal class...

Cited by 12 publications

References 59 publications

Synthetic Control over the Surface Chemistry of Blue-Emitting Perovskite Nanocrystals for Photocatalysis

Synthetic Control over the Surface Chemistry of Blue-Emitting Perovskite Nanocrystals for Photocatalysis

Mechanochemical synthesis of stable, quantum-confined CsPbBr3 perovskite nanocrystals with blue-green emission and high PLQY

Colloidal Metal‐Halide Perovskite Nanoplatelets: Thickness‐Controlled Synthesis, Properties, and Application in Light‐Emitting Diodes

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Mechanochemical synthesis of stable, quantum-confined CsPbBr₃ perovskite nanocrystals with blue-green emission and high PLQY