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Nat Commun. 2019 Aug 27;10(1):3872. doi: 10.1038/s41467-019-11887-2.

Multistep nucleation and growth mechanisms of organic crystals from amorphous solid states.

Author information

1
Beijing National Laboratory for Molecular Sciences, State Key Laboratory for Structural Chemistry of Unstable and Stable Species, College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871, P. R. China.
2
ICQD, Hefei National Laboratory for Physical Sciences at the Microscale, Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of Sciences, School of Physical Sciences, University of Science and Technology of China, Hefei, Anhui, 230026, P. R. China.
3
State Key Laboratory of Membrane Biology, Biomedical Pioneering Innovation Center, School of Life Sciences, Peking University, Beijing, 100871, P. R. China.
4
Beijing National Laboratory for Molecular Sciences, State Key Laboratory for Structural Chemistry of Unstable and Stable Species, College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871, P. R. China. junliang.sun@pku.edu.cn.
5
ICQD, Hefei National Laboratory for Physical Sciences at the Microscale, Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of Sciences, School of Physical Sciences, University of Science and Technology of China, Hefei, Anhui, 230026, P. R. China. wgzhu@ustc.edu.cn.
6
Beijing National Laboratory for Molecular Sciences, State Key Laboratory for Structural Chemistry of Unstable and Stable Species, College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871, P. R. China. guoxf@pku.edu.cn.
7
Department of Materials Science and Engineering, College of Engineering, Peking University, Beijing, 100871, P. R. China. guoxf@pku.edu.cn.

Abstract

Molecular self-assembly into crystallised films or wires on surfaces produces a big family of motifs exhibiting unique optoelectronic properties. However, little attention has been paid to the fundamental mechanism of molecular crystallisation. Here we report a biomimetic design of phosphonate engineered, amphiphilic organic semiconductors capable of self-assembly, which enables us to use real-time in-situ scanning probe microscopy to monitor the growth trajectories of such organic semiconducting films as they nucleate and crystallise from amorphous solid states. The single-crystal film grows through an evolutionary selection approach in a two-dimensional geometry, with five distinct steps: droplet flattening, film coalescence, spinodal decomposition, Ostwald ripening, and self-reorganised layer growth. These sophisticated processes afford ultralong high-density microwire arrays with high mobilities, thus promoting deep understanding of the mechanism as well as offering important insights into the design and development of functional high-performance organic optoelectronic materials and devices through molecular and crystal engineering.

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