Supracolloidal Self‐Assembly of Divalent Janus 3D DNA Origami via Programmable Multivalent Host/Guest Interactions

Abstract

We introduce divalent 3D DNA origami cuboids as truly monodisperse colloids and harness their ability for precision functionalization with defined patches and defined numbers of supramolecular binding motifs. We demonstrate that even adamantane/β‐cyclodextrin host/guest inclusion complexes of moderate association strength can induce efficient supracolloidal fibrillization at high dilution of the 3D DNA Origami as a result of cooperative multivalency. We show details on the assembly of Janus and non‐Janus 3D DNA origami into supracolloidal homo‐ and heterofibrils with respect to multivalency effects, electrostatic screening, and stoichiometry. We believe that the merger of 3D DNA origami with colloidal self‐assembly and supramolecular motifs provides new synergies at the interface of these disciplines to better understand multivalency effects, to promote structural complexity, and add non‐DNA assembling and switching mechanisms to DNA nanoscience.

Structural Deformation to β‐Cyclodextrin Due to Strong π‐Stacking in the Self‐Assembly of Inclusion Complex

“…The distortions are not transitory in nature and lead to formation of assemblies which are stable even at high temperatures. The structure and properties of cyclodextrins continue to inspire chemists [39–46] . In this context the understanding that CD structures are not inflexible may lead to design of novel molecular architectures in the future.…”

Self‐Propelling Janus Particles for Hemostasis in Perforating and Irregular Wounds with Massive Hemorrhage

“…To achieve this, the strategy of assembling the hybrid hemostatic particles would be extremely critical. The Janus particle, a widely applied catalyst and drug carrier, [22,23] is a typical micro-/nanoparticle with bipolar and heterogeneous structure that allows for two different types of chemistry on its surface. [24,25] Some Janus motors possess self-propelling properties caused by bubble detachment [26,27] ; once these Janus motors contact the specific fluid, they uniaxially release bubbles and propel themselves along a specific direction.…”

Dynamic spatial and structural organization in artificial cells regulates signal processing by protein scaffolding

“…1 Inspired by this biochemical logic, scientists from various disciplines have undertaken to mimic such systems and behaviors in synthetic analogs. [2][3][4][5][6][7] In this regard, self-assembled structures based upon peptides 8,9 or DNA [10][11][12][13][14] have been exemplary in how to program synthetic systems the way biology does; however, these systems do not display autonomous functionality. Contrary to most synthetic materials, living systems exhibit self-regulating and adaptable behavior that is maintained by dynamic (and transient) processes, where spatiotemporal regulation and organization of the ow of chemical information is critical.…”