Purcell Effect of Plasmonic Surface Lattice Resonances and Its Influence on Energy Transfer
Purcell Effect of Plasmonic Surface Lattice Resonances and Its Influence on Energy Transfer
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DOI：
10.1021/acsphotonics.1c00616
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发表时间：
2021-08-05
期刊：
影响因子：
7
通讯作者：
Menon, Vinod M.
中科院分区：
文献类型：
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作者：
Collison, Robert;Perez-Sanchez, Juan B.;Menon, Vinod M.
利用电磁模式设计光子态密度已经成为控制分子系统之间能量转移的一种有吸引力的方法。在这里，我们报告使用的表面晶格共振（SLR）中出现的阵列的金属-绝缘体-金属（MIM）nanocylinders控制两个原型分子染料，P580（供体）和P650（受体）之间的能量转移。当SLR与供体发射失谐时，如预期观察到能量转移，供体发射相对于受体发射降低（供体/受体峰值荧光比= 0.45）。相反，当SLR被调谐到供体发射时，珀塞尔增强变得占主导地位，胜过能量转移并抑制受体发射（供体/受体峰值荧光比=类似于5.4）。为了分析这些观测结果，开发了一个动力学模型，基于泵浦速率，供体-受体能量转移速率，以及染料的辐射和非辐射衰变。结果表明，由SLR引入的附加衰变通道，其中λ（SLR）（k平行于）= 0 = λ（供体）（发射）与能量转移过程强烈竞争，而与供体发射峰在较大的面内动量k（平行于）值处重合的SLR具有不太明显的效果。我们的研究突出了广泛的基于SLR的珀塞尔效应可能通过简单的晶格尺寸的变化和它们的后果在凝聚相的分子能量转移过程的动力学。
Engineering the density of photonic states with electromagnetic modes has become an attractive approach for controlling energy transfer between molecular systems. Here we report the use of surface lattice resonances (SLRs) that arise in arrays of metal-insulator-metal (MIM) nanocylinders to control the energy transfer between two archetypal molecular dyes, P580 ( donor) and P650 (acceptor). When the SLR is detuned from the donor emission, energy transfer is observed as expected, with donor emission decreasing with respect to the acceptor emission (donor/ acceptor peak fluorescence ratio = 0.45). In contrast, when the SLR is tuned to the donor emission, Purcell enhancement becomes dominant, outcompeting energy transfer and suppressing acceptor emission (donor/acceptor peak fluorescence ratio = similar to 5.4). To analyze these observations, a kinetic model was developed, based on pumping rate, donor-to-acceptor energy transfer rate, and radiative and nonradiative decay of the dyes. The results suggest the additional decay channel introduced by the SLR for which lambda(SLR)(k parallel to)= 0 = lambda(donor)(emission) competes strongly with the energy transfer process, while SLRs that coincide with donor emission peaks at larger values of in-plane momentum k(parallel to) have a less pronounced effect. Our study highlights the wide range of SLR-based Purcell effects possible by simple changes in the lattice dimensions and their consequences in the kinetics of molecular energy transfer processes in the condensed phase.