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Revealing Au13 as Elementary Clusters During the Early Formation of Au Nanocrystals

Journal Article · · Journal of Physical Chemistry Letters
 [1];  [2];  [3];  [1];  [3]
  1. BATTELLE (PACIFIC NW LAB)
  2. University of Michigan
  3. Zhejiang University
+ Show Author Affiliations

Understanding the formation mechanism of nanocrystals in solution is very fundamental to the development of materials science. For a metal nanocrystal, the cluster mediated formation mechanism is still poorly understood. Particularly, identifying what types of clusters are dominant and how they evolve into a nanocrystal in the early nucleation stage remains a great challenge. Here, using liquid-cell transmission electron microscopy, we directly observe the formation of ultra-small Au clusters (~0.84 nm) in the presence of PAA-Na. These clusters, which correspond to the size of Au13 cluster, coalesce to form nanocrystals. Our molecular dynamics simulations suggest Au13 in an aqueous environment have higher stability when compared to other cluster sizes and provide atomistic details of growth by cluster coalescence. Collectively, our demonstration of Au13 as the dominant species with elaboration of their coalescence kinetics sheds light on nonclassical nanocrystal formation mechanisms and offers useful guidelines for designing innovative pathways for synthesis of nanomaterials.

Research Organization:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Organization:
USDOE
DOE Contract Number:
AC05-76RL01830
OSTI ID:
1808788
Report Number(s):
PNNL-SA-164156
Journal Information:
Journal of Physical Chemistry Letters, Vol. 12, Issue 25
Country of Publication:
United States
Language:
English

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Related Subjects

Au13 clusters
cluster coalescence
liquid-cell TEM
nonclassical crystallization
PAA-Na