Two-Step Nanoparticle Crystallization via DNA-Guided Self-Assembly and the Nonequilibrium Dehydration Process

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DNA strands are powerful tools as ligand molecules that bind nanoparticles to each other via programmable self-assembly for colloidal crystallization. We found that hydrated DNA-functionalized nanoparticle (DNA-NP) superlattices with a properly controlled volume fraction and spatial arrangement of nanoparticles successfully maintained their crystallinity even after dehydration, which involves drastic contraction. A detailed study of the structural changes was performed for the self-assembled DNA-NP sample using small-angle X-ray scattering (SAXS) after dehydration. Then, an optimal volume fraction of nanoparticles in the superlattice, ϕ, which minimized the level of distortion of the dehydrated superlattice, was found for each bcc and fcc structure. By acquiring clear SAXS diffraction patterns showing crystal symmetries for dehydrated DNA-NP superlattices, their lattice distortion was evaluated using our analysis technique, which is based on Hosemann’s paracrystalline theory and involves SAXS and scanning electron microscopy data. Geometrical calculations substantiated the ease of movement of a nanoparticle under the influence of repulsions from adjacent particles that mainly affect the dehydration stability. These results suggest that it is possible to design the crystal structure of solid nanoparticle superlattices via DNA-guided nanoparticle assembly under a near-equilibrium state in solution as the first step, followed by dehydration under nonequilibrium conditions as the second step.

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