Two-step nanoparticle crystallization via DNA-guided self-assembly and non-equilibrium dehydration process
Two-step nanoparticle crystallization via DNA-guided self-assembly and non-equilibrium dehydration process
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通过 DNA 引导的自组装和非平衡脱水过程进行两步纳米颗粒结晶
DOI：
10.1021/acs.cgd.1c00398
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发表时间：
2021
影响因子：
3.8
通讯作者：
Miho Tagawa
中科院分区：
文献类型：
--
作者：
Hayato Sumi;Noboru Ohta;Hiroshi Sekiguchi;Shunta Harada;Toru Ujihara;Katsuo Tsukamoto;Miho Tagawa
DNA链是作为配体分子的强大工具，其通过可编程的自组装将纳米颗粒彼此结合以用于胶体结晶。我们发现，水合DNA功能化纳米粒子（DNA-NP）超晶格与适当控制的体积分数和空间排列的纳米粒子成功地保持其结晶度，即使在脱水后，这涉及剧烈收缩。利用小角X射线散射（SAXS）对脱水后的自组装DNA-NP样品的结构变化进行了详细的研究。然后，一个最佳的体积分数的纳米粒子在超晶格中，最大限度地减少了脱水的超晶格的变形的水平，被发现为每个bcc和fcc结构。通过获得清晰的SAXS衍射图显示脱水DNA-NP超晶格的晶体对称性，使用我们的分析技术，这是基于Hosemann的次晶理论，并涉及SAXS和扫描电子显微镜数据，其晶格畸变进行了评估。几何计算证实了从相邻的颗粒，主要影响脱水稳定性的排斥的影响下，纳米粒子的运动的容易性。这些结果表明，它是可能的设计固体纳米粒子超晶格的晶体结构，通过DNA引导的纳米粒子组装在溶液中的近平衡状态下作为第一步，然后在非平衡条件下脱水作为第二步。
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.