Department of Polymer Science and Engineering, State Key Laboratory of Coordination Chemistry, Key Laboratory of High Performance Polymer Materials and Technology of Ministry of Education, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, China.
Shanghai Key Laboratory of Advanced Polymeric Materials, School of Materials Science and Engineering, East China University of Science and Technology, Shanghai 200237, China.
J Phys Chem B. 2023 Sep 21;127(37):8049-8056. doi: 10.1021/acs.jpcb.3c04409. Epub 2023 Sep 12.
It is a challenging task to realize highly reversible ON-OFF nanoswitches over a wide range of temperatures, which emerge as a versatile toolbox for use in nanobiotechnology. Herein, nanoparticles (NPs) bifunctionalized by DNA strands and stimuli-responsive polymers are proposed to construct multimodal ON-OFF nanoswitches by the coarse-grained model. The successful achievement of multimodal ON-OFF nanoswitches for bifunctionalized NPs at lower temperatures is attributed to the synergistic effects of the contraction and expansion configurations of stimuli-responsive polymers, combined with the hybridization-dehybridization event of DNA strands. Importantly, our simulations isolate the conditions of programmable self-assembly of bifunctionalized NPs to realize the multimodal ON-OFF nanoswitches by the changes of temperature and chain rigidity. In addition, it is found that the bifunctionalized NPs in the ON state display anisotropic and patchy features due to an introduction of stimuli-responsive polymers. Our simulation results provide fundamental insights on qualitative predictions of ON/OFF states of DNA-based NPs, which can aid in realizing a set of ON-OFF nanoswitches by the rational design of functionalization molecules.
实现宽温度范围内高度可逆的 ON-OFF 纳米开关是一项具有挑战性的任务，它为纳米生物技术的应用提供了多功能工具。在此，通过粗粒度模型提出了由 DNA 链和响应性聚合物双功能化的纳米颗粒 (NPs)，以构建多模态的 ON-OFF 纳米开关。双功能化 NPs 的多模态 ON-OFF 纳米开关在较低温度下的成功实现归因于响应性聚合物的收缩和扩张构象以及 DNA 链的杂交-去杂交事件的协同作用。重要的是，我们的模拟通过温度和链刚性的变化来分离可编程自组装双功能化 NPs 的条件，以实现多模态 ON-OFF 纳米开关。此外，由于引入了响应性聚合物，处于 ON 状态的双功能化 NPs 显示出各向异性和斑片状特征。我们的模拟结果为基于 DNA 的 NPs 的 ON/OFF 状态的定性预测提供了基本的见解，这有助于通过功能化分子的合理设计实现一系列 ON-OFF 纳米开关。
