Revealing the Chiroptical Response of Plasmonic Nanostructures at the Nanofemto Scale.

The spatiotemporal origin of plasmonic chiroptical responses in nanostructures remains unexplored and unclear. Here, two orthogonally oriented Au nanorods as a prototype were investigated, with a giant chiroptical response caused by antisymmetric and symmetric mode excitations for obliquely incident left-handed circular polarization (LCP) and right-handed circular polarization (RCP) light. Time-resolved photoemission electron microscopy (PEEM) was employed to measure the near-field spatial distributions, spectra, and spatiotemporal dynamics of plasmonic modes associated with the chiroptical responses at the nanofemto scale, verifying the characteristic near-field distributions at the resonant wavelengths of the two modes and a very large spectral dichroism for LCP and RCP. More importantly, eigenmode excitations and their contributions to the ultrafast plasmonic chiroptical response in the space-time domain were directly revealed, promoting a full understanding of the ultrafast chiral origin in complex nanostructures. These findings open a way to design chiroptical nanophotonic devices for spatiotemporal control of chiral light-matter interactions.