Department of Physics and Astronomy, Queen Mary University of London, London, E1 4NS, United Kingdom.
Institute of Materials Research and Engineering (IMRE), Agency for Science, Technology and Research (A*STAR), 138634, Singapore.
Bioconjug Chem. 2023 Jan 18;34(1):78-84. doi: 10.1021/acs.bioconjchem.2c00285. Epub 2022 Aug 15.
The ability to control the assembly of mixed-dimensional heterostructures with nanoscale control is key for the fabrication of novel nanohybrid systems with new functionalities, particularly for optoelectronics applications. Herein we report a strategy to control the assembly of heterostructures and tune their electronic coupling employing DNA as a linker. We functionalized MoS nanosheets (NSs) with biotin-terminated dsDNA employing three different chemical strategies, namely, thiol, maleimide, and aryl diazonium. This allowed us to then tether streptavidinated quantum dots (QDs) to the DNA functionalized MoS surface via biotin-avidin recognition. Nanoscale control over the separation between QDs and NSs was achieved by varying the number of base pairs (bp) constituting the DNA linker, between 10, 20, and 30 bp, corresponding to separations of 3.4, 6.8, and 13.6 nm, respectively. Spectroscopic data confirmed the successful functionalization, while atomic force and transmission electron microscopy were employed to image the nanohybrids. In solution steady-state and time-resolved photoluminescence demonstrated the electronic coupling between the two nanostructures, that in turn was observed to progressively scale as a function of DNA linker employed and hence distance between the two nanomoieties in the hybrids.
用纳米级控制来控制混合维度异质结构的组装对于制造具有新功能的新型纳米杂化系统至关重要，特别是对于光电子应用。在此，我们报告了一种使用 DNA 作为连接物来控制异质结构组装并调整其电子耦合的策略。我们使用三种不同的化学策略，即巯基、马来酰亚胺和芳基重氮，将生物素化的双链 DNA 功能化到 MoS 纳米片 (NS) 上。这使我们能够通过生物素-亲和素识别将链霉亲和素化的量子点 (QD) 连接到 DNA 功能化的 MoS 表面。通过改变 DNA 连接子的碱基对 (bp) 数（分别为 10、20 和 30 bp，对应于 3.4、6.8 和 13.6 nm 的分离），实现了 QD 和 NS 之间分离的纳米级控制。光谱数据证实了成功的功能化，而原子力和透射电子显微镜则用于对纳米杂化物进行成像。在溶液稳态和时间分辨光致发光中证实了两种纳米结构之间的电子耦合，并且观察到电子耦合随着所使用的 DNA 连接子的变化以及在杂化物中两个纳米部分之间的距离而逐渐增加。
