论文标题

分子与表面等离子体之间的强耦合理论

Theory of strong coupling between molecules and surface plasmons on a grating

论文作者

Rider, Marie S, Arul, Rakesh, Baumberg, Jeremy J, Barnes, William L

论文摘要

分子与表面等离子体的强耦合导致杂种状态是部分分子,部分表面结合的光。由于分子共振可能会获得具有MM尺度传播长度的等离子的空间相干性,因此与分子共振的强耦合可能会启用远程分子能传递。光栅通常通过将原本非辐射的表面等离子体散射到光线内,将光滑的光线与表面等离子体相结合。当涉及光栅散射时,我们计算出与分子共振的表面等离子体的色散关系。通过将分子视为独立的振荡器,而不是更常见的单个集体偶极子,我们发现了完整的多波段分散关系。这种方法提供了一种自然的方式,将黑暗状态包括在色散中。我们证明,对于在向后和向后光栅散射的等离子体模式的交叉点附近调节的分子共振,等离子和分子之间的相互作用给出了五波段分散关系,包括使用单个集体偶极子的计算中未捕获的明亮状态。我们还表明,光栅在打破系统的翻译不变性中的作用出现在分子和表面等离子体之间的位置依赖性耦合中。因此,光栅的存在不仅对于分子表面 - 平面耦合的实验观察不仅重要,而且还提供了调谐系统的附加设计参数。

The strong coupling of molecules with surface plasmons results in hybrid states which are part molecule, part surface-bound light. Since molecular resonances may acquire the spatial coherence of plasmons, which have mm-scale propagation lengths, strong-coupling with molecular resonances potentially enables long-range molecular energy transfer. Gratings are often used to couple incident light to surface plasmons, by scattering the otherwise non-radiative surface plasmon inside the light-line. We calculate the dispersion relation for surface plasmons strongly coupled to molecular resonances when grating scattering is involved. By treating the molecules as independent oscillators rather than the more typically-considered single collective dipole, we find the full multi-band dispersion relation. This approach offers a natural way to include the dark states in the dispersion. We demonstrate that for a molecular resonance tuned near the crossing point of forward and backward grating-scattered plasmon modes, the interaction between plasmons and molecules gives a five-band dispersion relation, including a bright state not captured in calculations using a single collective dipole. We also show that the role of the grating in breaking the translational invariance of the system appears in the position-dependent coupling between the molecules and the surface plasmon. The presence of the grating is thus not only important for the experimental observation of molecule-surface-plasmon coupling, but also provides an additional design parameter that tunes the system.

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