期刊
NANO LETTERS
卷 20, 期 7, 页码 5001-5007出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.0c01125
关键词
magnetite; nanoparticles; nucleation; in situ SAXS/WAXS; classical nucleation theory; nonclassical crystallization
类别
资金
- French National Research Agency (ANR) [DIAMONS ANR-14-CE08-0003]
- ANR as part of the Investissements d'Avenir program [ANR-10-LABX-0035]
- Max Planck Society
- DFG (DFG-ANR) [FA 835/10-1]
- European Research Council [256915-MB2]
Crystallization from solution is commonly described by classical nucleation theory, although this ignores that crystals often form via disordered nanostructures. As an alternative, the classical theory remains widely used in a multistep variant, where the intermediate nanostructures merely introduce additional thermodynamic parameters. However, this variant still requires validation by experiments addressing indeed proper time and spatial scales (millisecond, nanometer). Here, we used in situ X-ray scattering to determine the mechanism of magnetite crystallization and, in particular, how nucleation propagates at the nanometer scale within amorphous precursors. We find that the self-confinement by an amorphous precursor slows down crystal growth by 2 orders of magnitude once the crystal size reaches the amorphous particle size (similar to 3 nm). Thus, not only the thermodynamic properties of transient amorphous nanostructures but also their spatial distribution determine crystal nucleation.
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