Dipartimento di Fisica, Sapienza Università di Roma , Piazzale A. Moro 2, 00185 Roma, Italy.
ACS Nano. 2014 Apr 22;8(4):3567-74. doi: 10.1021/nn501138w. Epub 2014 Mar 25.
Using state-of-the-art numerical techniques, we show that, upon lowering the temperature, tetravalent DNA nanostars form a thermodynamically stable, fully bonded equilibrium gel. In contrast to atomic and molecular network formers, in which the disordered liquid is always metastable with respect to some crystalline phase, we find that the DNA nanostar gel has a lower free energy than the diamond crystal structure in a wide range of concentrations. This unconventional behavior, here verified for the first time in a realistic model, arises from the large arm flexibility of the DNA nanostars, a property that can be tuned by design. Our results confirm the thermodynamic stability of the recently experimentally realized DNA hydrogels.
利用最先进的数值技术,我们表明,随着温度的降低,四价 DNA 纳米星会形成一种热力学稳定的、完全结合的平衡凝胶。与原子和分子网络形成物不同,在原子和分子网络形成物中,无序液体相对于某些晶体相总是亚稳的,我们发现 DNA 纳米星凝胶在很宽的浓度范围内具有比金刚石晶体结构更低的自由能。这种非传统的行为,在现实模型中首次得到验证,源于 DNA 纳米星的大臂灵活性,这种性质可以通过设计进行调整。我们的结果证实了最近实验实现的 DNA 水凝胶的热力学稳定性。