论文标题

等离激子纳米棒偶联染料分子的荧光增强

Mapping fluorescence enhancement of plasmonic nanorod coupled dye molecules

论文作者

Toth, Emese, Ungor, Ditta, Novak, Tibor, Ferenc, Gyorgyi, Banhelyi, Balazs, Csapo, Edit, Erdelyi, Miklos, Csete, Maria

论文摘要

血浆增强的荧光是经过广泛研究和应用现象,但是仅对偶联荧光团和等离子纳米孔子的比较理论和实验分析,才可以发现这种现象如何控制这种现象。将数值优化方法应用于能够增强激发和发射的设计构型,此外,在耦合的CY5染料分子和金纳米棒系统中同时同时构成了现象。参数灵敏度研究表明,荧光增强如何取决于分子的位置,距离和方向。专为同时改进而设计的耦合系统表现出最高(中间方向)的总荧光增强,伴随着对分子参数的中间敏感性,但激发波长的位置和方向敏感性除外。合成了与预测最佳构型相对应的几何形状的金纳米棒,并使用DNA链通过Cy5标记的寡核苷酸的杂交来控制距纳米棒表面的Cy5染料分子距离。最先进的DSTORM显微镜用于完成理论上预测(定向)总荧光增强的概念验证实验证明。测得的荧光增强与理论预测非常吻合,因此为设计和制备具有血浆增强荧光的耦合纳米系统提供了完整的套件。

Plasmonically enhanced fluorescence is a widely studied and applied phenomenon, however only a comparative theoretical and experimental analyses of coupled fluorophores and plasmonic nanoresonators makes it possible to uncover, how this phenomenon can be controlled. A numerical optimization method was applied to design configurations that are capable of resulting in an enhancement of excitation and emission, moreover of both phenomena simultaneously in coupled Cy5 dye molecule and gold nanorod systems. Parametric sensitivity studies revealed, how the fluorescence enhancement depends on the molecule's location, distance and orientation. Coupled systems designed for simultaneous improvement exhibited the highest (intermediate directional) total fluorescence enhancement, which is accompanied by intermediate sensitivity to the molecule's parameters, except the location and orientation sensitivity at the excitation wavelength. Gold nanorods with a geometry corresponding to the predicted optimal configurations were synthesized, and DNA strands were used to control the Cy5 dye molecule distance from the nanorod surface via hybridization of the Cy5-labelled oligonucleotide. State-of-the-art dSTORM microscopy was used to accomplish a proof-of-concept experimental demonstration of the theoretically predicted (directional) total fluorescence enhancement. The measured fluorescence enhancement was in good agreement with theoretical predictions, thus providing a complete kit to design and prepare coupled nanosystems exhibiting plasmonically enhanced fluorescence.

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