Journal
NATURE CHEMISTRY
Volume 9, Issue 1, Pages 77-82Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/NCHEM.2618
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Funding
- Singapore National Research Foundation's Competitive Research Program [NRF-CRP9-2011-04]
- National University of Singapore [NUSYIA-FY14-P17, 154-000-606-112]
- Microbiology Institute (Singapore)
- Centre for Bioimaging Sciences
- Lee Kuan Yew Endowment Fund
- National Science Foundation Division of Materials Research [1309765]
- American Chemical Society Petroleum Research Funding Grant [53062-ND6]
- [NRF-CRP8-2011-07]
- Direct For Mathematical & Physical Scien
- Division Of Materials Research [1309765] Funding Source: National Science Foundation
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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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