Microrheology of DNA hydrogels.

Microrheology of DNA hydrogels.
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DNA水凝胶的微观流变学

DOI:
10.1073/pnas.1722206115
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发表时间:
2018-08-07
影响因子:
11.1
通讯作者:
Eiser E
Eiser E
中科院分区:
综合性期刊1区
文献类型:
--
作者:
Xing Z;Caciagli A;Cao T;Stoev I;Zupkauskas M;O'Neill T;Wenzel T;Lamboll R;Liu D;Eiser E

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意义虽然广为人知的生命分子,DNA也是纳米尺度上令人惊叹的构建块,因为它允许我们设计和编程功能纳米材料的结构和动力学。我们利用DNA的可编程性来实现对自组装水凝胶的流变性的控制,这种水凝胶具有受温度精细调节的弹性或粘性行为(类似于黏液)。利用微观流变学研究DNA水凝胶在微长尺度上的力学性质,我们绘制了在广泛的频率和温度范围内的粘弹性响应。对基础物理的深入理解为设计基于DNA的材料提供了一种在分子水平上精确控制结构稳定性和刚性的方法。以DNA为基础的材料科学的一个关键目标是了解和精确控制DNA水凝胶的机械性能。我们使用扩散波谱(DWS)进行微观流变学测量,以研究由Y形DNA(Y-DNA)纳米星组成的水凝胶在广泛的频率和温度范围内的粘弹性行为。我们观察到在Y-DNA相互结合的熔化温度区域有一个明显的液体到凝胶的转变。我们的测量表明,弹性G‘(ω)和损耗模数G“(ω)之间存在交叉,这与体系的渗流转变相吻合。通过改变Y形状之间的DNA键长,可以很容易地改变这种转变的温度。利用整体流变学,我们进一步表明,通过降低Y-DNA键之间的柔性,我们可以在保持微观结构不变的情况下,从半柔性的瞬时网络转变为更具能量驱动、弹性更高的水凝胶。机械性能的这种控制水平将有助于设计更灵敏的分子传感工具和控制释放系统。
Significance While widely known as the molecule of life, DNA is also an amazing building block at the nanoscale, since it allows us to design and program the structure and dynamics of functional nanomaterials. We exploit the programmability of DNA to achieve control over the rheology of self-assembled hydrogels, which have elastic or viscous behavior (similar to that of slime) that is finely regulated by temperature. Using microrheology to investigate the mechanical properties of DNA hydrogels at the microlength scale, we map the viscoelastic response over a broad range of frequencies and temperatures. The deep understanding in the fundamental physics provides a way to design DNA-based materials with precise control over the structure stability and rigidity at molecular level. A key objective in DNA-based material science is understanding and precisely controlling the mechanical properties of DNA hydrogels. We perform microrheology measurements using diffusing wave spectroscopy (DWS) to investigate the viscoelastic behavior of a hydrogel made of Y-shaped DNA (Y-DNA) nanostars over a wide range of frequencies and temperatures. We observe a clear liquid-to-gel transition across the melting temperature region for which the Y-DNA bind to each other. Our measurements reveal a cross-over between the elastic G′(ω) and loss modulus G″(ω) around the melting temperature Tm of the DNA building blocks, which coincides with the systems percolation transition. This transition can be easily shifted in temperature by changing the DNA bond length between the Y shapes. Using bulk rheology as well, we further show that, by reducing the flexibility between the Y-DNA bonds, we can go from a semiflexible transient network to a more energy-driven hydrogel with higher elasticity while keeping the microstructure the same. This level of control in mechanical properties will facilitate the design of more sensitive molecular sensing tools and controlled release systems.
用于包裹和释放单细胞的触发式 DNA 水凝胶盖
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发表时间: 2013-09-14
期刊: ADVANCED MATERIALS
影响因子: 29.4
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发表时间: 1995-08-28
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影响因子: 5.5
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发表时间: 2009-01-01
期刊: PHYSICAL REVIEW E
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