In the study of the fabrication of DNA-templated silver nanoclusters （DNA-Ag NCs）, how templates affect the fluorescence of the nanoclusters remains undear, and it has been a challenge to understand the correlation ...In the study of the fabrication of DNA-templated silver nanoclusters （DNA-Ag NCs）, how templates affect the fluorescence of the nanoclusters remains undear, and it has been a challenge to understand the correlation between the properties of the DNA template and the Ag NCs. In this respect, based on the rational design of a series of structurally defined intramolecular G-quadruplexes, we prepared G-quadruplex-templated Ag NCs with a defined G-tetrad-to-silver ratio of 1：2. We evaluated the effect of G-quadruplex topology and loop sequences on the fluorescence of DNA-Ag NCs using circular dichroism, and extinction and emission spectroscopy. G-quadruplex templates with an anti-parallel topology were found to produce Ag NCs with stronger fluorescence compared with parallel and hybrid configurations. Loop bases adjacent to G-tetrads have a more significant impact on the fluorescence of Ag NCs compared with those in the middle of the loop, with adenine largely exhibiting an enhancement effect and thymine being detrimental. Generally, G-quadruplexes having an anti-parallel topology with adenine in the loop adjacent to the G-tetrad would be good templates for producing highly fluorescent Ag NCs. This is the first study to focus on the correlation between G-quadruplex topology/sequence and the optical properties of Ag NCs. We hope that the results of this study will facilitate a more in-depth understanding of correlation between G-quadruplex templates and Ag NCs, and help to understand and utilize their unique attributes.展开更多
基金This work was supported by the National Natural Science Foundation of China （Nos. 21535006, 21475004, and 21275011）.
文摘In the study of the fabrication of DNA-templated silver nanoclusters （DNA-Ag NCs）, how templates affect the fluorescence of the nanoclusters remains undear, and it has been a challenge to understand the correlation between the properties of the DNA template and the Ag NCs. In this respect, based on the rational design of a series of structurally defined intramolecular G-quadruplexes, we prepared G-quadruplex-templated Ag NCs with a defined G-tetrad-to-silver ratio of 1：2. We evaluated the effect of G-quadruplex topology and loop sequences on the fluorescence of DNA-Ag NCs using circular dichroism, and extinction and emission spectroscopy. G-quadruplex templates with an anti-parallel topology were found to produce Ag NCs with stronger fluorescence compared with parallel and hybrid configurations. Loop bases adjacent to G-tetrads have a more significant impact on the fluorescence of Ag NCs compared with those in the middle of the loop, with adenine largely exhibiting an enhancement effect and thymine being detrimental. Generally, G-quadruplexes having an anti-parallel topology with adenine in the loop adjacent to the G-tetrad would be good templates for producing highly fluorescent Ag NCs. This is the first study to focus on the correlation between G-quadruplex topology/sequence and the optical properties of Ag NCs. We hope that the results of this study will facilitate a more in-depth understanding of correlation between G-quadruplex templates and Ag NCs, and help to understand and utilize their unique attributes.
