论文标题

不可逆的聚合物凝结中的失控过渡与环化过渡

Runaway Transition in Irreversible Polymer Condensation with Cyclisation

论文作者

Panoukidou, Maria, Weir, Simon, Sorichetti, Valerio, Fosado, Yair Gutierrez, Lenz, Martin, Michieletto, Davide

论文摘要

聚合物凝结的过程,即反应性终端组之间的键形成,在行业和生物学中都是无处不在的。在这里,我们研究了在与环化竞争中经历聚合物凝结的通用系统。使用广义的Smoluchowski理论,使用DNA和T4连接酶的分子动力学模拟和实验,我们发现该系统显示出一个过渡,从无限时间的有限长度链的策略中,由环统治,并由一个由线性聚合物占主导地位的圆环,这些链被占主导地位。最后,我们表明,在大型凝结时间中,靠近过渡的流体可能具有明显不同的组成和流变学。

The process of polymer condensation, i.e. the formation of bonds between reactive end-groups, is ubiquitous in both industry and biology. Here we study generic systems undergoing polymer condensation in competition with cyclisation. Using a generalised Smoluchowski theory, molecular dynamics simulations and experiments using DNA and T4 ligase, we find that this system displays a transition, from a regime with finite-length chains at infinite time and dominated by rings to one dominated by linear polymers that grow in time. Finally, we show that fluids prepared close to the transition may have profoundly different compositions and rheology at large condensation times.

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