Optical field tuning of localized plasmon modes in Ag microcrystals at the nanofemto scale

Nanoscale plasmonic field enhancement at sub-wavelength metallic particles is crucial for surface sensitive spectroscopy, ultrafast microscopy, and nanoscale energy transduction. Here, we demonstrate control of the spatial distribution of localized surface plasmon modes at sub-optical-wavelength crystalline silver (Ag) micropyramids grown on a Si(001) surface. We employ multiphoton photoemission electron microscopy (mP-PEEM) to image how the plasmonic field distributions vary with the photon energy, light polarization, and phase in coherent two-pulse excitation. For photon energy hυ > 2.0 eV, the mP-PEEM images show single photoemission locus, which splits into a dipolar pattern that straddles the Ag crystal at a lower energy. We attribute the variation to the migration of plasmon resonances from the Ag/vacuum to the Ag/Si interfaces by choice of the photon energy. Furthermore, the dipolar response of the Ag/Si interface follows the polarization state of light: for linearly polarized excitations, the plasmon dipole follows the in-plane electric field vector, while for circularly polarized excitations, it tilts in the direction of the handedness due to the conversion of spin angular momentum of light into orbital angular momentum of the plasmons excited in the sample. Finally, we show the coherent control of the spatial plasmon distribution by exciting the sample with two identical circularly polarized light pulses with delay defined with attosecond precision. The near field distribution wobbles at the pyramid base as the pump-probe delay is advanced due to interferences among the contributing fields. We illustrate how the frequency, polarization, and pulse structure can be used to design and control plasmon fields on the nanofemto scale for applications in chemistry and physics.