论文标题

环线性DNA混合物的粘弹性特性表现出对混合组成的非单调依赖性

Viscoelastic properties of ring-linear DNA blends exhibit non-monotonic dependence on blend composition

论文作者

Peddireddy, K. R., Lee, M., Schroeder, C. M., Robertson-Anderson, R. M.

论文摘要

纠缠的环聚合物以及环和线性聚合物的混合物,由于文献中的实验结果相互矛盾,并且难以产生纠缠的合成环,而没有线性污染物,因此仍然是一个引起人们兴趣和辩论的话题。在这里,我们创建了纠缠环和线性DNA的混合溶液,线性DNA的质量分数变化。我们使用光学镊子微流变学来测量这些混合物的线性和非线性粘弹性响应。我们的测量结果揭示了线性粘弹性特性在线性DNA分数上具有强大的非单调依赖性,当环和线性链的质量分数可比性时,最大值的最大值,暗示了线性链通过线性链的泛滥螺纹。我们观察到非线性制度中类似的非单调性。但是,需要较高的线性链(0.5-0.7)的比例较高,即可大幅度增加复杂力和放松动力学的减慢。这种非线性响应似乎也取决于速率,我们认为这是由于力诱导的戒指以高应变速率的解读而引起的。我们的结果填补了有关环线性聚合物混合物的微流变学和非线性响应的长期差距。此外,环线性混合物所表现出的独特强烈的机械响应,以及通过改变混合组合物来精细调整这些混合物的能力,提供了新的材料设计原理。

Entangled ring polymers, along with blends of ring and linear polymers, continue to be a topic of great interest and debate due to the conflicting experimental results in the literature as well as the difficulty of producing entangled synthetic rings devoid of linear contaminants. Here, we create blended solutions of entangled ring and linear DNA with varying mass fractions of linear DNA. We use optical tweezers microrheology to measure the linear and nonlinear viscoelastic response of these blends. Our measurements reveal a strong non-monotonic dependence of linear viscoelastic properties on linear DNA fraction, with a pronounced maximum when the mass fraction of rings and linear chains are comparable, suggestive of pervasive threading of rings by linear chains. We observe a similar non-monotonicity in the nonlinear regime; however, a comparatively higher fraction of linear chains (0.5-0.7) is required for a substantial increase in resisitive force and slowing of relaxation dynamics to emerge. This nonlinear response also appears to be rate dependent, which we argue arises from force-induced de-threading of rings at high strain rates. Our results fill a longstanding gap in knowledge regarding the microrheology and nonlinear response of ring-linear polymer blends. Moreover, the uniquely strong mechanical response that ring-linear blends exhibit, along with the ability to finely tune these blends by varying the blend composition, provides new materials design principles.

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