Phase Behavior\nModulation of a Unary DNA Origami System\nthrough Allosteric Stimuli

A unary system is the most conceptually concise design\nfor conducting\nself-assembly. However, in most DNA-guided self-assembly schemes,\na unary system has rarely been adopted because of the inherent challenge\nof strictly decoupling the monomer synthesis process from the assembly\nprocess, which may directly lead to the inaccurate control over assembly.\nHerein, we provide a multi-stimulus-triggered assembly strategy based\non the DNA origami structure, which allows the unary system to realize\ncontrollable crystallization and phase transition by exerting allosteric\nstimuli. We intentionally introduced a specific DNA stimulus to convert\nthe self-aggregation of functionalized groups into the connection\nof nearby monomers, thus producing multidimensional high-quality crystals.\nFurthermore, this unary system can undergo a phase transition from\nsimple cubic to face-centered cubic with the introduction of more\ncation stimuli. We believe that this dynamic stimulation strategy\ncan offer a novel solution for fabricating materials with on-demand\nmodulation.