School of Chemistry and Chemical Engineering, State Key Laboratory of Metal Matrix Composites, Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai, 200240, China.
Key Laboratory of Flexible Electronics (KLOFE) &, Institute of Advanced Materials (IAM), Jiangsu National Synergetic Innovation Center for Advanced, Materials (SICAM), Nanjing Tech University (NJTECH), 30 South Puzhu Road, Nanjing, 211816, China.
Angew Chem Int Ed Engl. 2020 May 18;59(21):8133-8137. doi: 10.1002/anie.202000831. Epub 2020 Mar 18.
DNA-modified lanthanide-doped upconversion nanoparticles (DNA-UCNPs) that combine the functions of DNA and the optical features of UCNPs have shown great promise in a wide range of fields. However, challenges remain in precisely tethering and orienting the DNA strands on the UCNP surface. Herein, we systematically investigate the sequence dependence of DNAs in their interactions with UCNPs, and reveal that poly-cytosine (poly-C) has high affinity for the UCNP surface. A general approach to synthesize monodispersed DNA-UCNP conjugates is developed using poly-C-containing diblock DNA strands. The poly-C segment of the DNA strand binds to the surfaces of UCNPs and the second segment is oriented perpendicularly on the UCNP surface, making the DNA-UCNPs highly stable and monodispersed in aqueous solution. The dense layer of DNA on the UCNP surface enables the programmable assembly of UCNPs with other DNA-functionalized nanoparticles or DNA origamis through hybridization, resulting in the formation of well-organized complex structures.
DNA 修饰的镧系掺杂上转换纳米粒子（DNA-UCNPs）结合了 DNA 的功能和 UCNPs 的光学特性，在广泛的领域中显示出巨大的潜力。然而，在 UCNP 表面精确连接和定向 DNA 链仍然存在挑战。在此，我们系统地研究了 DNA 在与 UCNP 相互作用中的序列依赖性，并揭示了多胞嘧啶（poly-C）与 UCNP 表面具有高亲和力。使用含有多聚胞嘧啶的嵌段 DNA 链开发了一种合成单分散 DNA-UCNP 缀合物的通用方法。DNA 链的多聚-C 片段与 UCNP 表面结合，第二个片段在 UCNP 表面垂直取向，使 DNA-UCNPs 在水溶液中高度稳定且单分散。UCNP 表面上密集的 DNA 层使 UCNP 能够通过杂交与其他 DNA 功能化纳米粒子或 DNA 折纸结构进行可编程组装，从而形成组织良好的复杂结构。
