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Multistep nucleation of nanocrystals in aqueous solution

TitleMultistep nucleation of nanocrystals in aqueous solution
Publication TypeJournal Article
Year of Publication2017
AuthorsLoh, Duane N., Sen Soumyo, Bosman Michel, Tan Shu Fen, Zhong Jun, Nijhuis Christian A., Kral Petr, Matsudaira Paul, and Mirsaidov Utkur
JournalNat. Chem.
Date Published01/2017
Keywordsclusters, crystals, electron-microscopy, gold, growth, mechanisms, models, nanoclusters, nanoparticles, pathways

The nucleation and growth of solids from solutions impacts many natural processes and is fundamental to applications in materials engineering and medicine. For a crystalline solid, the nucleus is a nanoscale cluster of ordered atoms that forms through mechanisms still poorly understood. In particular, it is unclear whether a nucleus forms spontaneously from solution via a single-or multiple-step process. Here, using in situ electron microscopy, we show how gold and silver nanocrystals nucleate from supersaturated aqueous solutions in three distinct steps: spinodal decomposition into solute-rich and solute-poor liquid phases, nucleation of amorphous nanoclusters within the metal-rich liquid phase, followed by crystallization of these amorphous clusters. Our ab initio calculations on gold nucleation suggest that these steps might be associated with strong gold-gold atom coupling and water-mediated metastable gold complexes. The understanding of intermediate steps in nuclei formation has important implications for the formation and growth of both crystalline and amorphous materials.


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