Towards Active Self-Assembly Through DNA Nanotechnology.

Self-assembly, which is ubiquitous in living systems, also stimulates countless synthetic molecular self-assembling systems. Most synthetic self-assemblies are realized by passive processes, going from high-energy states to thermodynamic equilibrium. Conversely, living systems work out of equilibrium, meaning they are energy-consuming, dissipative and active. In recently years, chemists have made extensive efforts to design artificial active self-assembly systems, which will be pivotal to emulating and understanding life. Among various strategies, emerging approaches based on DNA nanotechnology have attracted a lot of attention. Structural- as well as dynamic-DNA-nanotechnology offer diverse tools with which to design building blocks and to shape their assembly behaviors. To achieve active self-assembly, a synergy of diverse DNA techniques is essential, including structural design, controllable assembly-disassembly, autonomous assembly, molecular circuits, biochemical oscillators, and so on. In this review, we introduce progress towards, or related to, active assembly via DNA nanotechnology. Dynamic DNA assembly systems ranging from passive assembly-disassembly systems, to autonomous assembly systems to sophisticated artificial metabolism and time-clocking oscillation systems will be discussed. We catalogue these systems from the perspective of free energy change with the reaction process. We end the review with a brief outlook and discussion.