Selective excitation of a three-dimensionally oriented single plasmonic dipole

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.

Cylindrical vector beam-excited frequency-tunable second harmonic generation in a plasmonic octamer

We report a method to tune the second harmonic generation(SHG) frequency of a metallic octamer by employing cylindrical vector beams as the excitation. Our method exploits the ability to spatially match the polarization state of excitations with the fundamental target plasmonic modes, enabling flexible control of the SHG resonant frequency.It is found that SHG of the octamer is enhanced over a broad band(400 nm) by changing the excitation from the linearly polarized Gaussian beam to radially and azimuthally polarized beams. More strikingly, when subjected to an azimuthally polarized beam, the SHG intensity of the octamer becomes 30 times stronger than that for the linearly polarized beam even in the presence of Fano resonance.