Plasmon-coupled resonance energy transfer: A real-time electrodynamics approach

Plasmon-coupled resonance energy transfer: A real-time electrodynamics approach
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DOI:
10.1063/1.4975815
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发表时间:
2017-02-14
影响因子:
4.4
通讯作者:
Schatz, George C.
Schatz, George C.
中科院分区:
化学2区
文献类型:
--
作者:
Ding, Wendu;Hsu, Liang-Yan;Schatz, George C.

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本文提出了一种新的实时电动力学方法,用于确定在等离子体或其他纳米结构(非均匀吸收和色散介质)的存在下,两个分子之间的共振能量转移(RET)的速率。在这种等离子体激元耦合共振能量转移(PC-RET)方法中,我们开发了能量转移矩阵元素的经典电动力学表达式,使用时域有限差分(FDTD)方法求解分子供体产生的电场的麦克斯韦方程并在分子受体的位置进行评估。我们证明,这种方法产生RET率在均匀介质中,是在精确的协议与基于量子电动力学(QED)的分析理论。在金纳米粒子的存在下,我们的理论表明,远程衰减的RET率可以显着修改等离子体激元激发,与率增加多达106倍,导致能量转移率超过数百纳米的纳米相比,在几十纳米的纳米粒子的情况下。这些有前途的结果表明,重要的未来应用的PC-RET领域涉及光捕获或传感,其中涉及不均匀的吸收和色散介质的能量转移过程是司空见惯的。出版社:AIP Publishing
This paper presents a new real-time electrodynamics approach for determining the rate of resonance energy transfer (RET) between two molecules in the presence of plasmonic or other nanostructures (inhomogeneous absorbing and dispersive media). In this approach to plasmon-coupled resonance energy transfer (PC-RET), we develop a classical electrodynamics expression for the energy transfer matrix element which is evaluated using the finite-difference time-domain (FDTD) method to solve Maxwell's equations for the electric field generated by the molecular donor and evaluated at the position of the molecular acceptor. We demonstrate that this approach yields RET rates in homogeneous media that are in precise agreement with analytical theory based on quantum electrodynamics (QED). In the presence of gold nanoparticles, our theory shows that the long-range decay of the RET rates can be significantly modified by plasmon excitation, with rates increased by as much as a factor of 106 leading to energy transfer rates over hundreds of nm that are comparable to that over tens of nm in the absence of the nanoparticles. These promising results suggest important future applications of the PC-RET in areas involving light harvesting or sensing, where energy transfer processes involving inhomogeneous absorbing and dispersive media are commonplace. Published by AIP Publishing.