期刊
NATURE MATERIALS
卷 16, 期 7, 页码 767-+出版社
NATURE PUBLISHING GROUP
DOI: 10.1038/NMAT4891
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- US Department of Energy, Office of Basic Energy Sciences, Biomolecular Materials Program at Pacific Northwest National Laboratory (PNNL)
- Lawrence Livermore National Laboratory
- Department of Energy by Battelle [DE-AC05-76RL01830]
- US Department of Energy [DE-AC52-07NA27344]
Two-step nucleation pathways in which disordered, amorphous, or dense liquid states precede the appearance of crystalline phases have been reported for a wide range of materials, but the dynamics of such pathways are poorly understood. Moreover, whether these pathways are general features of crystallizing systems or a consequence of system-specific structural details that select for direct versus two-step processes is unknown. Using atomic force microscopy to directly observe crystallization of sequence-defined polymers, we show that crystallization pathways are indeed sequence dependent. When a short hydrophobic region is added to a sequence that directly forms crystalline particles, crystallization instead follows a two-step pathway that begins with the creation of disordered clusters of 10-20 molecules and is characterized by highly non-linear crystallization kinetics in which clusters transform into ordered structures that then enter the growth phase. The results shed new light on non-classical crystallization mechanisms and have implications for the design of self-assembling polymer systems.
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