Multistep nucleation of nanocrystals in aqueous solution

N. Duane Loh, Soumyo Sen, Michel Bosman, Shu Fen Tan, Jun Zhong, Christian A. Nijhuis*, Petr Kral, Paul Matsudaira, Utkur Mirsaidov

*Corresponding author for this work

Research output: Contribution to journalArticleAcademicpeer-review

185 Citations (Scopus)
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Abstract

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.
Original languageEnglish
Pages (from-to)77-82
JournalNature chemistry
Volume9
Issue number1
DOIs
Publication statusPublished - Jan 2017
Externally publishedYes

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