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.
Keywords: DNA nanotechnology; chemical reaction network; chiral metamolecules; plasmonic; transient self-assembly.