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Probing the Mechanisms of Strong Fluorescence Enhancement in Plasmonic Nanogaps with Sub-nanometer Precision
ACS Nano ( IF 15.8 ) Pub Date : 2020-10-23 , DOI: 10.1021/acsnano.0c01973 Boxiang Song 1 , Zhihao Jiang 2 , Zerui Liu 1 , Yunxiang Wang 1 , Fanxin Liu 3 , Stephen B. Cronin 1 , Hao Yang 1 , Deming Meng 1 , Buyun Chen 1 , Pan Hu 1 , Adam M. Schwartzberg 4 , Stefano Cabrini 4 , Stephan Haas 2 , Wei Wu 1
ACS Nano ( IF 15.8 ) Pub Date : 2020-10-23 , DOI: 10.1021/acsnano.0c01973 Boxiang Song 1 , Zhihao Jiang 2 , Zerui Liu 1 , Yunxiang Wang 1 , Fanxin Liu 3 , Stephen B. Cronin 1 , Hao Yang 1 , Deming Meng 1 , Buyun Chen 1 , Pan Hu 1 , Adam M. Schwartzberg 4 , Stefano Cabrini 4 , Stephan Haas 2 , Wei Wu 1
Affiliation
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Plasmon-enhanced fluorescence is demonstrated in the vicinity of metal surfaces due to strong local field enhancement. Meanwhile, fluorescence quenching is observed as the spacing between fluorophore molecules and the adjacent metal is reduced below a threshold of a few nanometers. Here, we introduce a technology, placing the fluorophore molecules in plasmonic hotspots between pairs of collapsible nanofingers with tunable gap sizes at sub-nanometer precision. Optimal gap sizes with maximum plasmon enhanced fluorescence are experimentally identified for different dielectric spacer materials. The ultrastrong local field enhancement enables simultaneous detection and characterization of sharp Raman fingerprints in the fluorescence spectra. This platform thus enables in situ monitoring of competing excitation enhancement and emission quenching processes. We systematically investigate the mechanisms behind fluorescence quenching. A quantum mechanical model is developed which explains the experimental data and will guide the future design of plasmon enhanced spectroscopy applications.
中文翻译：
用亚纳米精度探索等离子体纳米间隙中强荧光增强的机理
由于强烈的局部电场增强，在金属表面附近显示出等离子体增强的荧光。同时，随着荧光团分子与相邻金属之间的间隔减小到几纳米的阈值以下，观察到了荧光猝灭。在这里，我们介绍一种技术，将荧光团分子放置在成对的可折叠纳米指之间的等离激元热点中，间隙大小可调至亚纳米精度。对于不同的介电间隔物材料，实验确定了具有最大等离激元增强荧光的最佳间隙尺寸。超强的局部电场增强功能可同时检测和表征荧光光谱中的尖锐拉曼指纹。因此，该平台可实现原位监测竞争性激发增强和发射猝灭过程。我们系统地研究了荧光猝灭的机制。开发了量子力学模型，该模型解释了实验数据，并将指导等离激元增强光谱学应用的未来设计。
更新日期：2020-11-25
中文翻译：
用亚纳米精度探索等离子体纳米间隙中强荧光增强的机理
由于强烈的局部电场增强，在金属表面附近显示出等离子体增强的荧光。同时，随着荧光团分子与相邻金属之间的间隔减小到几纳米的阈值以下，观察到了荧光猝灭。在这里，我们介绍一种技术，将荧光团分子放置在成对的可折叠纳米指之间的等离激元热点中，间隙大小可调至亚纳米精度。对于不同的介电间隔物材料，实验确定了具有最大等离激元增强荧光的最佳间隙尺寸。超强的局部电场增强功能可同时检测和表征荧光光谱中的尖锐拉曼指纹。因此，该平台可实现原位监测竞争性激发增强和发射猝灭过程。我们系统地研究了荧光猝灭的机制。开发了量子力学模型，该模型解释了实验数据，并将指导等离激元增强光谱学应用的未来设计。
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