Extended Nucleation and Superfocusing in Colloidal Semiconductor Nanocrystal Synthesis

Prins, P. Tim; Montanarella, Federico; Dümbgen, Kim; Justo, Yolanda; Bok, Johanna C. van der; Hinterding, Stijn; Geuchies, Jaco J.; Maes, Jorick; Nolf, Kim De; Deelen, Sander; Meijer, Hans; Zinn, Thomas; Петухов, А.В.; Rabouw, Freddy T.; Donegá, Celso de Mello; Vanmaekelbergh, Daniël; Hens, Zeger

doi:10.1021/acs.nanolett.0c04813

Cited by 43 publications

(70 citation statements)

References 63 publications

(135 reference statements)

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“…In the end, a new mechanism for the formation of InP QDs is proposed, by which growth is dictated by the surface reactivity of the QDs. Similar behavior has recently been highlighted in the well-established CdSe hot-injection synthesis …”

Section: Introductionsupporting

confidence: 79%

Size-Controlled Indium Phosphide Quantum Dots for Bright and Tunable Light Emission by Simple Hindered Diamine Addition

Valleix

Cisnetti

Okuno

et al. 2021

ACS Appl. Nano Mater.

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The use of sterically hindered N,N′-diisopropylbenzene-1,2-diamine (DIBA) for aminophosphine-based InP QDs synthesis in an oleylamine (OLAm) medium is evidenced as a powerful tool to finely control their size in a reproducible way. This diamine forms in situ a P(DIBA)(OLAm) species accounting for the observed size-tuning effect because the QDs crystallize as tetrahedra with an edge length (3.5 to 6.6 nm) depending on the DIBA concentration (0 to 7 eq./indium). This kinetically controlled size-tuning mechanism is proposed by combining 31 P NMR and UV−vis spectroscopy. A proof-of-concept is established by coating the InP cores with ZnS shells. The luminescence of the as-synthesized InP/ZnS QDs is tunable over the 480−620 nm range, with photoluminescence internal quantum efficiencies of 45 to 60% suitable for applications as phosphors in LED lighting systems and LED displays.

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Section: Introductionsupporting

confidence: 79%

Size-Controlled Indium Phosphide Quantum Dots for Bright and Tunable Light Emission by Simple Hindered Diamine Addition

Valleix

Cisnetti

Okuno

et al. 2021

ACS Appl. Nano Mater.

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“…These calculated values match well with the values of a = 1.84 nm determined from the absorption spectrum of the cores and b = 4.1 ± 0.4 nm (mean ± standard deviation) from electron microscopy (red arrows in Figure b). A dominant contribution of variations in the CdSe/CdS core–shell size b to inhomogeneous broadening could be expected on the basis of our synthesis procedure and those of many others. ,, For the core synthesis, growth is fast and is stopped before size defocusing of a sets in . Shells, on the other hand, are grown at a low growth rate to avoid secondary nucleation, which may lead to Ostwald ripening effects that widen the distribution of shell thicknesses …”

mentioning

confidence: 88%

Biexciton Binding Energy and Line width of Single Quantum Dots at Room Temperature

et al. 2021

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Broadening of multiexciton emission from colloidal quantum dots (QDs) at room temperature is important for their use in high-power applications, but an in-depth characterization has not been possible until now. We present and apply a novel spectroscopic method to quantify the biexciton line width and biexciton binding energy of single CdSe/CdS/ZnS colloidal QDs at room temperature. In our method, which we term “cascade spectroscopy”, we select emission events from the biexciton cascade and reconstruct their spectrum. The biexciton has an average emission line width of 86 meV on the single-QD scale, similar to that of the exciton. Variations in the biexciton repulsion (E b = 4.0 ± 3.1 meV; mean ± standard deviation of 15 QDs) are correlated with but are more narrowly distributed than variations in the exciton energy (10.0 meV standard deviation). Using a simple quantum-mechanical model, we conclude that inhomogeneous broadening in our sample is primarily due to variations in the CdS shell thickness.

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“…[ 192 ] In HI, the precursor is injected while the reaction mixture is heated to a set temperature, and the reaction is stopped by cooling. [ 1,193 ] The cooling rate can influence the size and size distribution of the resulting nanoparticles. An alternative approach is ligand‐assisted reprecipitation (LARP), which is similar to HI, but the reaction mixture is quenched by the addition of an antisolvent.…”

Section: Monitoring Of Synthesis In Batch Reactorsmentioning

confidence: 99%

Importance of Monitoring the Synthesis of Light‐Interacting Nanoparticles – A Review on In Situ, Ex Situ, and Online Time‐Resolved Studies

Pinho

Zhang

Hoye

et al. 2022

Advanced Optical Materials

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Reducing the dimensionality of materials from bulk thin films and single crystals to nanocrystals (NCs) and quantum dots This review paper analyzes the importance of monitoring the synthesis of plasmonic and optoelectronic materials to provide a mechanistic understanding of their nucleatiçon and growth, as well as crucial kinetic insights to enable their future development. Light-interacting nanoparticles present strong size-property relationships, such that size control is at the core of any synthetic development. However, conventional ex situ characterization of these materials has heavily limited their development to simple trial-and-error approaches. Over the last decade, the development of in situ and online characterization capabilities has transformed the understanding of mechanistic models. In addition, time-resolved data are able to reveal the step rate, even for phenomena taking place in the microsecond timescale (i.e., nucleation), thanks to the use of micro-flow-reactors. However, the literature contains a few disagreements and inaccuracies, which are considered to be due to the general lack of attention and control on mixing (relevant when mixing time is comparable to the reaction time), and the presence of additives during synthesis (e.g., stabilizers). Finally, it is believed that recent in situ monitoring development coupled with reactor design brings unique opportunities to not only synthesize nanoparticles in a reproducible and controllable manner, but also gives data-rich approaches for self-regulated and automated systems.

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Extended Nucleation and Superfocusing in Colloidal Semiconductor Nanocrystal Synthesis

Cited by 43 publications

References 63 publications

Size-Controlled Indium Phosphide Quantum Dots for Bright and Tunable Light Emission by Simple Hindered Diamine Addition

Size-Controlled Indium Phosphide Quantum Dots for Bright and Tunable Light Emission by Simple Hindered Diamine Addition

Biexciton Binding Energy and Line width of Single Quantum Dots at Room Temperature

Importance of Monitoring the Synthesis of Light‐Interacting Nanoparticles – A Review on In Situ, Ex Situ, and Online Time‐Resolved Studies

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