Man Tiantian, Ji Wei, Liu Xiaoguo, Zhang Chuan, Li Li, Pei Hao, Fan Chunhai
Shanghai Key Laboratory of Green Chemistry and Chemical Processes, School of Chemistry and Molecular Engineering , East China Normal University , 500 Dongchuan Road , Shanghai 200241 , People's Republic of China.
School of Chemistry and Chemical Engineering , Shanghai Jiao Tong University , Shanghai 200240 , People's Republic of China.
ACS Nano. 2019 Apr 23;13(4):4826-4833. doi: 10.1021/acsnano.9b01942. Epub 2019 Apr 10.
Energy-dissipating self-assembly is at the basis of many important cellular processes, such as cell organization, proliferation, and morphogenesis. Beyond equilibrium self-assembled molecular systems and materials, it is increasingly recognized that the control of assembly kinetics provides great opportunity for the next generation of molecular materials with intelligent behavior including programmed spatiotemporal organization. Here we show the transient self-assembly of active chiral plasmonic metamolecules (CPMs), which is controlled by the proton flux generated from a positive-feedback chemical reaction network. The fuel-conversion kinetics allows for temporal control and adaptive tuning of multiple structures of plasmonic metamolecules (PMs). This approach enables autonomous tuning of chiroptical properties of metamolecules with dynamic behavior. Moreover, we show that 11 types of spatial configurations of PMs are assembled, and 9 types of temporal configurations of CPMs are differentiated.
能量耗散自组装是许多重要细胞过程的基础，如细胞组织、增殖和形态发生。除了平衡自组装分子系统和材料外，人们越来越认识到，控制组装动力学为具有智能行为（包括程序化时空组织）的下一代分子材料提供了巨大机遇。在此，我们展示了活性手性等离子体超分子（CPM）的瞬态自组装，其由正反馈化学反应网络产生的质子通量控制。燃料转换动力学允许对等离子体超分子（PM）的多种结构进行时间控制和自适应调节。这种方法能够自主调节具有动态行为的超分子的手性光学性质。此外，我们展示了PM的11种空间构型被组装，以及CPM的9种时间构型被区分。
