Probing Surface Plasmon Dynamics in Periodic Nanostructures through Ultrafast Electron Microscopy

Surface plasmon polaritons (SPPs) can be manipulated to localize and guide light in subwavelength distances, enabling them to find applications in a wide range of areas, from sensing to quantum computing. Among several methods of SPP excitation, periodic arrays of nano- and microstructures are of particular interest, as they enable engineering SPP properties through structural parameters. Here, using the photon-induced near-field electron microscopy (PINEM) technique, we investigated the mode formation, coupling, interference, and decay of SPPs in square and hexagonal arrays of circular nanoholes under both visible and near-infrared excitation. Polarization-resolved analysis revealed the key factors governing SPP localization and interference patterns, showing that the periodicity and symmetry of the array primarily determine the SPP interference patterns and their orientation, while pump polarization mainly modulates their intensity. Time-resolved PINEM measurements demonstrated the spatial dependence of the SPP temporal characteristics. In addition, cathodoluminescence (CL) spectroscopy was employed to examine the intrinsic plasmonic characteristics of the structure. Finite difference time domain (FDTD) simulations showed strong agreement with both PINEM and CL measurements on the spatial and spectral behavior of SPPs. Understanding the spatiotemporal dynamics of SPPs on nanostructures beyond the diffraction limit is crucial for optimizing plasmonic structures for advanced photonic and quantum technologies.