Cencini Aura, Bortoluzzi Mary, Rilievo Graziano, Tonolo Federica, Vianello Fabio, Magro Massimiliano, Cecconello Alessandro
Department of Comparative Biomedicine and Food Science, University of Padua, Viale dell'Università 16, 35020 Legnaro, PD, Italy.
Int J Mol Sci. 2025 Mar 12;26(6):2557. doi: 10.3390/ijms26062557.
DNA is an exceptional building block for the fabrication of dynamic supramolecular systems with switchable geometries. Here, a self-assembled, tunable plasmonic-fluorescent nanostructure was developed. A precise sliding motion mechanism was operated through the control of strand displacement reactions, shifting two single-strand DNA (ssDNA) rails connected by a ssDNA quasi-ring structure. The system was reconfigured as a nano-mechanical structure, generating six discrete configurations, and setting specific distances between a tethered gold nanoparticle (AuNP) and a fluorophore, Sulfo-Cyanine3 (Cy3). Each configuration produced a distinct fluorescence emission intensity via plasmonic quenching/enhancement effects, and therefore the structure behaved as a nano-ruler. To optimize the system, the reversible distance-dependent fluorescence quenching or enhancement phenomena were investigated by testing AuNPs with diameters of 5, 10, and 15 nm, yielding the best performances with 10 nm AuNPs. Furthermore, a geometric model of the system was produced, confirming the observed results. The fluorophore-plasmonic surface positioning, conferred by the DNA ruler, led to a finite state nano-machine with six alternative signal outputs. This mechanism, working as a fluorescent reporter, could find application in a multiple-responsive detection system of single-strand nucleic acids, such as viruses or microRNAs.
DNA是用于构建具有可切换几何形状的动态超分子系统的特殊构建模块。在此,开发了一种自组装的、可调节的等离子体荧光纳米结构。通过控制链置换反应来操作精确的滑动运动机制,移动由单链DNA(ssDNA)准环结构连接的两条单链DNA(ssDNA)轨道。该系统被重新配置为一种纳米机械结构,产生六种离散构型,并在连接的金纳米颗粒(AuNP)和荧光团磺化菁3(Cy3)之间设定特定距离。每种构型通过等离子体猝灭/增强效应产生独特的荧光发射强度,因此该结构表现为一把纳米尺。为了优化该系统,通过测试直径为5、10和15 nm的AuNP研究了可逆的距离依赖性荧光猝灭或增强现象,结果表明10 nm的AuNP具有最佳性能。此外,还建立了该系统的几何模型,证实了观察结果。由DNA尺赋予的荧光团-等离子体表面定位导致了一种具有六种交替信号输出的有限状态纳米机器。这种作为荧光报告器的机制可应用于单链核酸(如病毒或微小RNA)的多重响应检测系统。