Department of Chemical Sciences and Technologies, University of Rome, Tor Vergata, Via della Ricerca Scientifica, 00133 Rome, Italy.
Molecular Biophysics Group, Peter Debye Institute for Soft Matter Physics, Universität Leipzig, 04103 Leipzig, Germany.
J Am Chem Soc. 2023 Sep 27;145(38):20968-20974. doi: 10.1021/jacs.3c06664. Epub 2023 Sep 14.
Inspired by naturally occurring regulatory mechanisms that allow complex temporal pulse features with programmable delays, we demonstrate here a strategy to achieve temporally programmed pulse output signals in DNA-based strand displacement reactions (SDRs). To achieve this, we rationally designed input strands that, once bound to their target duplex, can be gradually degraded, resulting in a pulse output signal. We also designed blocker strands that suppress strand displacement and determine the time at which the pulse reaction is generated. We show that by controlling the degradation rate of blocker and input strands, we can finely control the delayed pulse output over a range of 10 h. We also prove that it is possible to orthogonally delay two different pulse reactions in the same solution by taking advantage of the specificity of the degradation reactions for the input and blocker strands. Finally, we show here two possible applications of such delayed pulse SDRs: the time-programmed pulse decoration of DNA nanostructures and the sequentially appearing and self-erasing formation of DNA-based patterns.
受自然界中调节机制的启发,这些机制允许具有可编程延迟的复杂时间脉冲特征,我们在此展示了一种在基于 DNA 的链置换反应(SDR)中实现时间编程脉冲输出信号的策略。为了实现这一点,我们合理设计了输入链,一旦与靶双链结合,这些输入链就可以逐渐降解,从而产生脉冲输出信号。我们还设计了阻断链来抑制链置换并确定产生脉冲反应的时间。我们表明,通过控制阻断链和输入链的降解速率,可以在 10 小时的范围内精细控制延迟脉冲输出。我们还证明,通过利用输入链和阻断链的降解反应的特异性,在同一溶液中正交延迟两个不同的脉冲反应是可行的。最后,我们展示了这种延迟脉冲 SDR 的两种可能应用:DNA 纳米结构的时间编程脉冲装饰和基于 DNA 的图案的顺序出现和自我擦除形成。