Can Nanocavities Significantly Enhance Resonance Energy Transfer in a Single Donor–Acceptor Pair?
Can Nanocavities Significantly Enhance Resonance Energy Transfer in a Single Donor–Acceptor Pair?
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DOI：
10.1021/acs.jpcc.1c04623
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发表时间：
2021-08
期刊：
影响因子：
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通讯作者：
Yu-Chen Wei;Ming-Wei Lee;Pi‐Tai Chou;G. Scholes;G. Schatz;Liang-Yan Hsu
中科院分区：
文献类型：
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作者：
Yu-Chen Wei;Ming-Wei Lee;Pi‐Tai Chou;G. Scholes;G. Schatz;Liang-Yan Hsu
在过去的几十年里，纳米尺度上的长程共振能量转移（RET）和能量转移的控制在实验和理论上都受到了相当大的关注。我们已经研究了在纳米腔中的施主/受主对之间的RET基于我们以前的理论发展的宏观量子电动力学（QED）的框架。在此理论基础上，计算了法布里-珀罗腔在真空条件下RET随速率的增强。当两个分子之间的位移矢量与法布里-珀罗腔的腔轴对齐时，我们发现腔模由于共振和非共振腔模的贡献之间的干涉而产生小于10倍的增强。通过比较，当两个分子之间的位移矢量在垂直于腔轴的平面内对齐时，我们发现腔模式可以诱导超过10倍的增强，并且表面等离子体激元极化激元模式可以诱导高达300倍的增强。我们开发了一个方便的表示理解分子之间的位移矢量和分子偶极方向的H-二聚体和J-二聚体的性质的影响。为了进一步提高RET，我们提出了一个正方形的银腔，在腔谐振条件下，给出了280倍的速率增强，这提供了重要的洞察力开发设备能够远程RET。
Long-range resonance energy transfer (RET) and the control of energy transfer on the nanoscale have received considerable attention both experimentally and theoretically during the past few decades. We have investigated the RET between a donor/acceptor pair in the nanocavities based on our previous theory developed in the framework of macroscopic quantum electrodynamics (QED). On the basis of this theory, the enhancements in the RET with respect to the rate in vacuum were evaluated for a Fabry–Pérot cavity. When the displacement vector between the two molecules is aligned with the cavity axis of the Fabry–Pérot cavity, we find that cavity modes give enhancements of less than a factor of 10 due to the interference between contributions from resonant and non-resonant cavity modes. By comparison, when the displacement vector between the two molecules is aligned in a plane perpendicular to the cavity axis, we find that the cavity modes can induce enhancements of more than a factor of 10, and the surface plasmon-polariton modes can induce enhancements of up to a factor of 300. We develop a convenient representation for understanding the effect of the displacement vector between the molecules and of the molecular dipole directions in terms of the H-dimer and J-dimer properties. To further enhance the RET, we propose a square silver cavity that gives a rate enhancement of a factor of 280 under cavity resonance conditions, which provides important insight into developing devices capable of long-range RET.