4.8 Article

Growth of Colloidal Nanocrystals by Liquid-Like Coalescence**

Journal

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 60, Issue 12, Pages 6667-6672

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202014275

Keywords

coalescence; growth kinetics; nanoparticles; nanostructures; Smoluchowski' s model

Funding

  1. MSR-Intel program of Semiconductor Research Corporation [2015-IN-2582]

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This study describes, models, and predicts the growth kinetics of amine-capped PbS colloidal nanoparticles in the absence of supersaturation. The nanoparticles grow by coalescence rather than Ostwald ripening, with low activation energy attributed to differences in particle size and suppression of collision rates between rare populations. The model successfully predicts nanoparticle growth kinetics, enabling precise control of average particle size without the need for supersaturation.
We here describe, model, and predict the growth kinetics of amine-capped PbS colloidal nanoparticles in the absence of supersaturation. The particles grow by coalescence rather than by Ostwald ripening. A comparison of different models indicates that the effective activation energy of coalescence (67.65 kJ mol(-1)) is associated with two terms: a term proportional to the contact area between the ligand shells of two colliding particles, and a constant term. Our Brownian dynamics simulations show (i) how the remarkably low activation energy (or large rate constants) are most likely due to the large difference in size between the particles and their mean free path of diffusion, and (ii) how the low polydispersity is the likely result of the suppression of collision rates between rare populations due to crowding. The model successfully predicts the growth kinetics of nanoparticles, therefore enabling the precise control of the average particle size without the need of supersaturation.

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