表面等离激元因其极强的束缚光场能力，成为亚波长尺度下研究光与物质相互作用的理想平台，也是构建未来小型化、低功耗、高便携光电子器件的核心单元。更多维度、更加精确和灵活地调控等离激元的模式性质对推动其基础和应用研究至关重要。近年来，光场调控技术的发展，拓展了人们利用光场的维度，也赋予光场更强大的操控等离激元模式的能力。本文简述了矢量光场与等离激元模式作用的基本理论与物理机制，回顾了近年来矢量光场调控等离激元模式激发、耦合和远场辐射的研究进展，并介绍了相关研究在增强光谱、纳米颗粒光捕获、纳米位移传感等方面的应用。

We experimentally demonstrate a scheme to deterministically excite a three-dimensionally oriented electric dipole in a single Au nanosphere by using a tightly focused radially polarized beam whose focal field possesses polarization states along three-dimensional (3D) orientations owing to the spatial overlap between longitudinal and radial electric field components. Experiment observations indicate that the orientation of an excited dipole moment gradually changes from out-of-plane to in-plane when the nanosphere is moved away from the beam center, which is reconfirmed by full-wave simulations. Moreover, rigorous calculation based on Mie theory reveals that a reduced effective ambient permittivity accompanies the rotation of the dipole moment, leading to a blue-shifted and narrowed resonance peak. We envision that our results could find applications in detecting the 3D orientation of isolated molecules and benefit the fine manipulation of light–matter interactions at the single-molecule level.