Model-Based Insight into Single-Molecule Plasmonic Mislocalization
Model-Based Insight into Single-Molecule Plasmonic Mislocalization
复制标题
基于模型的单分子等离子体错位洞察
DOI：
10.1021/acs.jpcc.1c07989
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发表时间：
2021
期刊：
影响因子：
--
通讯作者：
Biteen, Julie S.
中科院分区：
文献类型：
--
作者：
Zuo, Tiancheng;Goldwyn, Harrison J.;Masiello, David J.;Biteen, Julie S.
贵金属纳米颗粒充当可见波长天线，重塑附近染料分子的发射。因为单分子成像克服了系综平均，所以它特别适合于理解这些等离子体效应。我们设计了由ATTO590染料分子包围的金纳米盘组成的单粒子组件，并通过双链DNA连接物连接。这些组件提供了一个可控的几何结构，将等离子体耦合染料分子放置在纳米盘平面上的特定径向位置，并为进一步分析提供了真实的染料分子位置。我们将分子-纳米天线相互作用建模为两个耦合偶极子，并通过衍射限制显微镜传播它们的干涉场，以产生耦合偶极子图像，准确地再现了在等离子体增强单分子荧光数值模拟中看到的扭曲psf。我们将模拟和实验数据拟合到模型函数以及标准高斯函数中，并评估了模型方法的优点。总的来说，我们发现图像模型可以更好地重现染料分子错误定位的某些方面，并且我们提出可以通过将高阶等离子体多极效应集成到纳米盘响应中以及同时使用图像和光谱信息来解决剩余的空白。
Noble metal nanoparticles act as visible-wavelength antennas that reshape the emission of nearby dye molecules. Because single-molecule imaging overcomes ensemble averaging, it is uniquely suited for understanding these plasmonic effects. We have engineered single-particle assemblies consisting of a gold nanodisk surrounded by ATTO590 dye molecules attached by double-stranded DNA linkers. These assemblies provide a controlled geometry that places plasmon-coupled dye molecules at specific radial positions in the plane of the nanodisk and provides the ground truth actual dye molecule position for further analysis. We modeled the molecule–nanoantenna interaction as two coupled dipoles and propagated their interfering fields through a diffraction-limited microscope to generate a coupled-dipole image that accurately recreates the distorted PSFs seen in numerical simulations of plasmon-enhanced single-molecule fluorescence. We fit simulated and experimental data to the model function as well as to a standard Gaussian function and evaluated the advantages of the model approach. Overall, we find that the image model can better recapture certain aspects of the dye molecule mislocalization, and we propose that remaining gaps can be addressed by integrating higher-order plasmon multipole effects into the nanodisk response as well as by simultaneously using both image and spectral information.
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作者：
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