Crystallization of Nanocrystals in Spherical Confinement Probed by in Situ X-ray Scattering.

Montanarella, Federico; Geuchies, Jaco J; Dasgupta, Tonnishtha; Prins, P Tim; van Overbeek, Carlo; Dattani, Rajeev; Baesjou, Patrick; Dijkstra, Marjolein et al. · Nano Lett · 2018

basic_science · Level V

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Abstract

We studied the formation of supraparticles from nanocrystals confined in slowly evaporating oil droplets in an oil-in-water emulsion. The nanocrystals consist of an FeO core, a CoFe<sub>2</sub>O<sub>4</sub> shell, and oleate capping ligands, with an overall diameter of 12.5 nm. We performed in situ small- and wide-angle X-ray scattering experiments during the entire period of solvent evaporation and colloidal crystallization. We observed a slow increase in the volume fraction of nanocrystals inside the oil droplets up to 20%, at which a sudden crystallization occurs. Our computer simulations show that crystallization at such a low volume fraction is only possible if attractive interactions between colloidal nanocrystals are taken into account in the model as well. The spherical supraparticles have a diameter of about 700 nm and consist of a few crystalline face-centered cubic domains. Nanocrystal supraparticles bear importance for magnetic and optoelectronic applications, such as color tunable biolabels, color tunable phosphors in LEDs, and miniaturized lasers.