Plasmonic wavelength-dependent optical switch.

We design and experimentally demonstrate an optical switch based on the interference of plasmonic modes in whispering gallery mode (WGM) antennas. Simultaneous excitation of even and odd WGM modes, enabled by a small symmetry breaking via non-normal illumination, allows switching the plasmonic near field between opposite sides of the antenna, depending on the excitation wavelength used in a wavelength range of 60 nm centered around 790 nm. This proposed switching mechanism is experimentally demonstrated by combining photoemission electron microscopy (PEEM) with a tunable wavelength femtosecond laser source in the visible and infrared.

Coherent response of the electronic system driven by non-interfering laser pulses.

The strength of light-matter interaction in condensed matter is fundamentally linked to the orientation and oscillation strength of the materials' optical transition dipoles. Structurally anisotropic materials, e.g., elongated molecules, exhibit optical transition dipoles with fixed orientations that govern the angular-dependent light-matter interaction. Contrary, free electron-like metals should exhibit isotropic light-matter interaction with the light fields dictating the orientation of the optical transition dipoles. Here, we demonstrate that an anisotropic direction of the optical transition dipoles even exists in highly free electron-like noble metal surfaces. Our time- and phase-resolved photoemission experiment reveals coherent interference effects on the (110)-oriented silver surface after optical excitation with two non-interfering cross-polarized pulses. We explain this coherent material response within the density matrix formalism by an intrinsic coupling of the non-interfering light fields mediated by optical transition dipoles with fixed orientations in silver.

Energy and Momentum Distribution of Surface Plasmon-Induced Hot Carriers Isolated via Spatiotemporal Separation.

Understanding the differences between photon-induced and plasmon-induced hot electrons is essential for the construction of devices for plasmonic energy conversion. The mechanism of the plasmonic enhancement in photochemistry, photocatalysis, and light-harvesting and especially the role of hot carriers is still heavily discussed. The question remains, if plasmon-induced and photon-induced hot carriers are fundamentally different or if plasmonic enhancement is only an effect of field concentration producing these carriers in greater numbers. For the bulk plasmon resonance, a fundamental difference is known, yet for the technologically important surface plasmons, this is far from being settled. The direct imaging of surface plasmon-induced hot carriers could provide essential insight, but the separation of the influence of driving laser, field-enhancement, and fundamental plasmon decay has proven to be difficult. Here, we present an approach using a two-color femtosecond pump-probe scheme in time-resolved 2-photon-photoemission (tr-2PPE), supported by a theoretical analysis of the light and plasmon energy flow. We separate the energy and momentum distribution of the plasmon-induced hot electrons from that of photoexcited electrons by following the spatial evolution of photoemitted electrons with energy-resolved photoemission electron microscopy (PEEM) and momentum microscopy during the propagation of a surface plasmon polariton (SPP) pulse along a gold surface. With this scheme, we realize a direct experimental access to plasmon-induced hot electrons. We find a plasmonic enhancement toward high excitation energies and small in-plane momenta, which suggests a fundamentally different mechanism of hot electron generation, as previously unknown for surface plasmons.

Spectroscopic Evidence for a New Type of Surface Resonance at Noble-Metal Surfaces.

We investigated the surface and bulk properties of the pristine (110) surface of silver using threshold photoemission by excitation with light of 5.9 eV. Using a momentum microscope, we identified two distinct transitions along the Γ[over ¯]Y[over ¯] direction of the crystal. The first one is a so far unknown surface resonance of the (110) noble-metal surface, exhibiting an exceptionally large bulk character that has so far been elusive in surface sensitive experiments. The second one stems from the well-known bulklike Mahan cone oriented along the ΓL direction inside the crystal but projected onto the (110)-surface cut. The existence of the new state is confirmed by photocurrent calculations, and its character is analyzed.

Near-field mechanism of the enhanced broadband magneto-optical activity of hybrid Au loaded Bi:YIG.

We unravel the underlying near-field mechanism of the enhancement of the magneto-optical activity of bismuth-substituted yttrium iron garnet films (Bi:YIG) loaded with gold nanoparticles. The experimental results show that the embedded gold nanoparticles lead to a broadband enhancement of the magneto-optical activity with respect to the activity of the bare Bi:YIG films. Full vectorial near- and far-field simulations demonstrate that this broadband enhancement is the result of a magneto-optically enabled cross-talking of orthogonal localized plasmon resonances. Our results pave the way to the on-demand design of the magneto-optical properties of hybrid magneto-plasmonic circuitry.