Dynamic Interface-Assisted Rapid Self-Assembly of DNA Origami-Framed Anisotropic Nanoparticles

Abstract

The ordered arrangement of nanoparticles can generate unique physicochemical properties, rendering it a pivotal direction in the field of nanotechnology. DNA-based chemical encoding has emerged as an unparalleled strategy for orchestrating precise and controlled nanoparticle assemblies. Nonetheless, it is often time-consuming and has limited assembly efficiency. In this study, we developed a strategy for the rapid and ordered assembly of DNA origami-framed nanoparticles assisted by dynamic interfaces. By assembling Au nanoparticles (AuNPs) onto DNA origami with different sticky ends in various directions, we endowed them with anisotropic specific affinities. After assembling DNA origami-framed AuNPs onto supported lipid bilayers with freely diffusing single-stranded DNA via DNA hybridization, we found that DNA origami-framed AuNPs could form larger ordered assemblies than those in 3D solution within equivalent time frames. Furthermore, we also achieved rapid and ordered assembly of liposome nanoparticles by employing the aforementioned strategy. Our work provides a novel avenue for efficient and rapid assembly of nanoparticles across two-dimensional interfaces, which is expected to promote the application of ordered nanoparticle assemblies in sensor and biomimetic system construction.

Figure 1

Schematic showing the design of triangular DNA origami Units 1 and 2 (a) and 2D dynamic interface (SLBs)-assisted rapid self-assembly of Units 1 and 2. Chol-ssDNA: cholesterol-modified ssDNA.

Figure 2

(a,b) Atomic force microscopy imaging results of the self-assembly of Units 1 and 2 on the SLBs (a) and representative height maps of 1D DNA origami arrays (b). (c) Atomic force microscopy imaging results of the self-assembly of Units 1 and 2 in a solution environment. (d) Histogram of the frequency distribution of the number of DNA origami units in self-assembled structures under different conditions. (e,f) TIRFM imaging results of the self-assembly of Units 1 and 2 on the SLBs (e) and in solution (f). Scale bar is 200 nm in parts a and c; scale bar is 3 μm in parts e and f.

Figure 3

(a) Schematic showing the design of DNA origami-framed AuNPs, and representative AFM images showing the self-assembly of Unit 1- and Unit 2-framed AuNPs. (b,c) TIRFM imaging demonstrating the self-assembly of Unit 1- and Unit 2-framed 15 nm AuNPs (b) and 30 nm AuNPs (c) on SLBs at different time points. Scale bars in b and c are 2 and 1 μm, respectively.

Figure 4

(a) Schematic showing the design of DNA origami-framed liposomes and their self-assembly. (b) TIRFM imaging demonstrating the self-assembly of Unit 1- and Unit 2-framed liposome on SLB at different time point. Scale bar: 2 μm.