Leaving Forster Resonance Energy Transfer Behind: Nanometal Surface Energy Transfer Predicts the Size-Enhanced Energy Coupling between a Metal Nanoparticle and an Emitting Dipole
Leaving Forster Resonance Energy Transfer Behind: Nanometal Surface Energy Transfer Predicts the Size-Enhanced Energy Coupling between a Metal Nanoparticle and an Emitting Dipole
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DOI：
10.1021/jp407259r
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发表时间：
2013-11-14
影响因子：
3.7
通讯作者：
Strouse, Geoffrey F.
中科院分区：
文献类型：
--
作者：
Breshike, Christopher J.;Riskowski, Ryan A.;Strouse, Geoffrey F.
荧光分子与金纳米颗粒的相互作用是复杂的，并且可以导致激发态增强或淬灭。许多人试图解释在金属表面附近观察到的相互作用，但没有一个单一的模型能够解释这些观察结果。在这项工作中，我们表明，通过准确地描述的相互作用的诱导图像偶极子内修改的金纳米粒子的吸收率和介电常数的大小依赖性的变化，振荡器的相互作用可以完全描述在表面调节的相互作用。实验和理论数据的比较证实了所选范围的分离距离，纳米粒子半径和荧光分子选择的模型的有效性。该研究的结果说明了非辐射途径的重要性，通过耦合到图像偶极子修改荧光分子的衰变，从而提供了一个坚实的理解报告的变化行为的发射物种在接近纳米金属表面。结果的一个更重要的影响是应用纳米金属表面能量转移方法作为分子标尺的能力，以探测比以前更大的距离（>400埃）的物理问题。
The interaction of a fluorescent molecule with a gold nanoparticle is complex and can lead to excited-state enhancement or quenching. Many attempts have been made to explain the observed interaction when in close proximity to the metal surface; yet no single model has been capable of explaining the observations. In this work, we show that by accurately describing the interaction in terms of an induced image dipole modified within the gold nanoparticle by the size-dependent changes in absorptivity and dielectric constant, the oscillator interaction can be fully described in terms of a surface-moderated interaction. Comparison of experimental and theoretical data confirms the validity of the model for a selected range of separation distances, nanoparticle radii, and fluorescent molecule selection. The results of the study illustrate the importance of nonradiative pathways for modifying the decay of a fluorescent molecule by coupling to the image dipole, thus providing a firm understanding of the reported variance in behavior for an emitting species in close proximity to nanometal surfaces. A more significant impact of the results is the ability to apply nanometal surface energy transfer methods as a molecular ruler to probe physical questions at much greater distances (>400 angstrom) than previously achievable.