论文标题
DNA功能化纳米颗粒的自组装中热力学与动力学之间的相互作用
The interplay between thermodynamics and kinetics in the self-assembly of DNA functionalized nanoparticles
论文作者
论文摘要
我们使用DNA官能化颗粒的粗粒模型来了解DNA链长度在其自组装中的作用。我们发现，给定粒径的链长的增加会降低形成有序结晶组件的倾向，而当链长超过一定阈值时，无序结构开始形成，这与先前的实验一致。对模拟数据的进一步分析表明，随着链长的增加削弱了颗粒间相互作用，从而将合适的组装条件转移到较低的温度下，在该温度下，组装动力学不利。这突出了热力学和动力学之间的复杂相互作用，我们建议可以通过更改系统参数（例如DNA移植密度）进行调节，从而成功地结晶了具有更长的DNA链长度的颗粒。我们的结果突出了计算建模在阐明基本设计原理并指导纳米颗粒组装以形成复杂纳米结构的力量。
We use a coarse-grained model of DNA-functionalized particles to understand the role of DNA chain length on their self-assembly. We find that the increasing chain length for a given particle size decreases the propensity to form ordered crystalline assemblies, and instead, disordered structures start to form when the chain length exceeds a certain threshold, which is consistent with the previous experiments. Further analysis of the simulation data suggests weakening interparticle interactions with increasing chain length, thereby shifting the suitable assembly conditions to lower temperatures at which assembly dynamics are unfavorable. This highlights a complex interplay between thermodynamics and dynamics, which we suggest can be modulated by changing the system parameters such as DNA grafting density, resulting in successful crystallization of particles with longer DNA chain lengths. Our results highlight the power of computational modeling in elucidating the fundamental design principles and guiding the assembly of nanoparticles to form complex nanostructures.
