Breaking translational symmetry via polymer chain overcrowding in molecular bottlebrush crystallization

Hao Qi, Xiting Liu, Daniel M. Henn, Shan Mei, Mark C. Staub, Bin Zhao () and Christopher Y. Li ()
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Hao Qi: Drexel University
Xiting Liu: Drexel University
Daniel M. Henn: University of Tennessee
Shan Mei: Drexel University
Mark C. Staub: Drexel University
Bin Zhao: University of Tennessee
Christopher Y. Li: Drexel University

Nature Communications, 2020, vol. 11, issue 1, 1-9

Abstract: Abstract One of the fundamental laws in crystallization is translational symmetry, which accounts for the profound shapes observed in natural mineral crystals and snowflakes. Herein, we report on the spontaneous formation of spherical hollow crystals with broken translational symmetry in crystalline molecular bottlebrush (mBB) polymers. The unique structure is named as mBB crystalsome (mBBC), highlighting its similarity to the classical molecular vesicles. Fluorescence resonance energy transfer (FRET) experiments show that the mBBC formation is driven by local chain overcrowding-induced asymmetric lamella bending, which is further confirmed by correlating crystalsome size with crystallization temperature and mBBʼs side chain grafting density. Our study unravels a new principle of spontaneous translational symmetry breaking, providing a general route towards designing versatile nanostructures.

Date: 2020
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DOI: 10.1038/s41467-020-15477-5

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