Institute of Physics and Center of Interface Science, Carl von Ossietzky University, Oldenburg, Germany.
Centre for Nanoscience and Nanotechnology (C2N), CNRS, Université Paris-Sud, Université Paris-Saclay, Palaiseau, France.
Nat Nanotechnol. 2019 Jul;14(7):698-704. doi: 10.1038/s41565-019-0441-y. Epub 2019 May 13.
The coherent exchange of optical near fields between two neighbouring dipoles plays an essential role in the optical properties, quantum dynamics and thus the function of many naturally occurring and artificial nanosystems. These interactions are challenging to quantify experimentally. They extend over only a few nanometres and depend sensitively on the detuning, dephasing and relative orientation (that is, the vectorial properties) of the coupled dipoles. Here, we introduce plasmonic nanofocusing spectroscopy to record coherent light scattering spectra with 5 nm spatial resolution from the apex of a conical gold nanotaper. The apex is excited solely by evanescent fields and coupled to plasmon resonances in a single gold nanorod. We resolve resonance energy shifts and line broadenings as a function of dipole distance and relative orientation. We demonstrate how these phenomena arise from mode couplings between different vectorial components of the interacting optical near fields, specifically from the coupling of the nanorod to both transverse and longitudinal polarizabilities of the taper apex.
两个邻近偶极子之间光近场的相干交换在许多自然发生和人工纳米系统的光学性质、量子动力学以及功能中起着至关重要的作用。这些相互作用很难在实验上进行量化。它们的作用范围只有几纳米,并且对耦合偶极子的失谐、退相和相对取向(即矢量特性)非常敏感。在这里,我们引入等离子体纳米聚焦光谱学,从锥形金纳米锥的顶点记录具有 5nm 空间分辨率的相干光散射光谱。顶点仅由消逝场激发,并与单个金纳米棒中的等离子体共振耦合。我们解析了共振能量位移和线宽随偶极子距离和相对取向的变化。我们展示了这些现象如何源于相互作用光近场不同矢量分量之间的模式耦合,特别是纳米棒与锥顶点的横向和纵向极化率的耦合。