ATP-powered molecular recognition to engineer transient multivalency and self-sorting 4D hierarchical systems.

Nature Communications
Jie Deng, Andreas Walther

Abstract

Biological systems organize multiple hierarchical structures in parallel, and create dynamic assemblies and functions by energy dissipation. In contrast, emerging artificial non-equilibrium self-assembling systems have remained relatively simplistic concerning hierarchical design, and non-equilibrium multi-component systems are uncharted territory. Here we report a modular DNA toolbox allowing to program transient non-equilibrium multicomponent systems across hierarchical length scales by introducing chemically fueled molecular recognition orchestrated by reaction networks of concurrent ATP-powered ligation and cleavage of freely programmable DNA building blocks. Going across hierarchical levels, we demonstrate transient side-chain functionalized nucleic acid polymers, and further introduce the concept of transient cooperative multivalency as a key to bridge length scales to pioneer fuel-driven encapsulation, self-assembly of colloids, and non-equilibrium transient narcissistic colloidal self-sorting on a systems level. The fully programmable and functionalizable DNA components pave the way to design chemically fueled 4D (3 space, 1 time) molecular multicomponent systems and autonomous materials.

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Citations

Mar 24, 2021·Journal of the American Chemical Society·Zhixin ZhouItamar Willner
Mar 9, 2021·Angewandte Chemie·Xinlong Fan, Andreas Walther
Apr 18, 2021·The New Phytologist·Olga Speck, Thomas Speck
Mar 5, 2021·Biofabrication·Guy DecanteJ Miguel Oliveira
Jun 15, 2021·Biophysics and Physicobiology·Yusuke Sato, Yuki Suzuki
Jul 2, 2021·Materials Today. Bio·O Burgos-MoralesW Weber
Aug 3, 2021·Journal of the American Chemical Society·Chen WangItamar Willner
Aug 11, 2021·Nature Chemistry·Felix J RizzutoHanadi F Sleiman
Jul 13, 2021·Angewandte Chemie·Mehak Jain, Bart Jan Ravoo
Dec 17, 2020·Journal of the American Chemical Society·Jie Deng, Andreas Walther

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Methods Mentioned

BETA
electrophoresis
FRET
fluorescence spectroscopy

Software Mentioned

DySS
ImageJ

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