Till Leißner

Spatiotemporal Characterization of SPP Pulse Propagation in Two-Dimensional Plasmonic Focusing Devices

The spatiotemporal evolution of a SPP wave packet with femtosecond duration is experimentally investigated in two different plasmonic focusing structures. A two-dimensional reconstruction of the plasmonic field in space and time is possible by the numerical analysis of interferometric time-resolved photoemission electron microscopy data. We show that the time-integrated and time-resolved view onto the wave packet dynamics allow one to characterize and compare the capabilities of two-dimensional components for use in plasmonic devices operating with ultrafast pulses.

Mapping surface plasmon polariton propagation via counter-propagating light pulses

In an interferometric time-resolved photoemission electron microscopy (ITR-PEEM) experiment, the near-field associated with surface plasmon polaritons (SPP) can be locally sensed via interference with ultrashort laser pulses. Here, we present ITR-PEEM data of SPP propagation at a gold vacuum interface recorded in a counter-propagating pump-probe geometry. In comparison to former work this approach provides a very intuitive real-time access to the SPP wave packet. The quantitative analysis of the PEEM data enables us to determine in a rather direct manner the propagation characteristics of the SPP.

The Interplay between Localized and Propagating Plasmonic Excitations Tracked in Space and Time

In this work, the mutual coupling and coherent interaction of propagating and localized surface plasmons within a model-type plasmonic assembly is experimentally demonstrated, imaged, and analyzed. Using interferometric time-resolved photoemission electron microscopy the interplay between ultrashort surface plasmon polariton wave packets and plasmonic nanoantennas is monitored on subfemtosecond time scales. The data reveal real-time insights into dispersion and localization of electromagnetic fields as governed by the elementary modes determining the functionality of plasmonic operation units.

Surface Plasmon Polariton Emission Prompted by Organic Nanofibers on Thin Gold Films

The excitation of surface plasmon polaritons (SPP) at a gold–vacuum interface by femtosecond light pulses mediated by organic nanofiber-induced dielectric perturbations is observed using interferometric time-resolved photoemission electron microscopy. The experimental data are quantitatively reproduced by analytic simulations, where the nanofibers are considered as superior source of the SPP emission. The flexibility and tuneability of phenylene-based nanofibers in their morphology and intrinsic optical properties open up future applications to fabricate custom-designed nanoscale sources of SPP.

Surface plasmon polariton propagation in organic nanofiber based plasmonic waveguides.

Plasmonic wave packet propagation is monitored in dielectric-loaded surface plasmon polariton waveguides realized from para-hexaphenylene nanofibers deposited onto a 60 nm thick gold film. Using interferometric time resolved two-photon photoemission electron microscopy we are able to determine phase and group velocity of the surface plasmon polariton (SPP) waveguiding mode (0.967c and 0.85c at λ(Laser) = 812nm) as well as the effective propagation length (39 μm) along the fiber-gold interface. We furthermore observe that the propagation properties of the SPP waveguiding mode are governed by the cross section of the waveguide.

Measurement of surface plasmon autocorrelation functions

In this paper we demonstrate the realization of an autocorrelator for the characterization of ultrashort surface plasmon polariton (SPP) pulses. A wedge shaped structure is used to continuously increase the time delay between two interfering SPPs. The autocorrelation signal is monitored by non-linear two-photon photoemission electron microscopy. The presented approach is applicable to other SPP sensitive detection schemes that provide only moderate spatial resolution and may therefore be of general interest in the field of ultrafast plasmonics.

Nanostructure induced changes in lifetime and enhanced second-harmonic response of organic-plasmonic hybrids

In this letter we show that the optical response of organic nanofibers, grown from functionalized para-quaterphenylene molecules, can be controlled by forming organic-plasmonic hybrid systems. The interaction between nanofibers and supporting regular arrays of nanostructures leads to a strongly enhanced second harmonic response. At the same time, the fluorescence lifetime of the nanofibers is reduced from 0.32 ns for unstructured gold films to 0.22 ns for gold nanosquare arrays, demonstrating efficient organic–plasmonic interaction. To study the origin of these effects, we applied two-photon laser scanning microscopy and fluorescence lifetime imaging microscopy. These findings provide an effective approach for plasmon-enhanced second-harmonic generation at the nanoscale, which is attractive for nanophotonic circuitry.

Surface plasmons excited by the photoluminescence of organic nanofibers in hybrid plasmonic systems

Recent research on hybrid plasmonic systems has shown the existence of a loss channel for energy transfer between organic materials and plasmonic/metallic structured substrates. This work focuses on the exciton-plasmon coupling between para-Hexaphenylene (p-6P) organic nanofibers (ONFs) and surface plasmon polaritons (SPPs) in organic/dielectric/metal systems. We have transferred the organic p-6P nanofibers onto a thin silver film covered with a dielectric (silicon dioxide) spacer layer with varying thicknesses. Coupling is investigated by two-photon fluorescence-lifetime imaging microscopy (FLIM) and leakage radiation spectroscopy (LRS). Two-photon excitation allows us to excite the ONFs with near-infrared light and simultaneously avoids direct SPP excitation on the metal layer. We observe a strong dependence of fluorescence lifetime on the type of underlying substrate and on the morphology of the fibers. The experimental findings are complemented via finite-difference time-domain (FDTD) modeling. The presented results lead to a better understanding and control of hybrid-mode systems, which are crucial elements in future low-loss energy transfer devices.

Local field enhanced second-harmonic response of organic nanofibers deposited on encapsulated plasmonic substrates

In this work, enhancement of the second harmonic response of organic nanofibers deposited on encapsulated and robust plasmonic active substrate is experimentally demonstrated. Organic nanofibers grown from functionalized paraquaterphenylene (CNHP4) molecules have been transferred on lithographically defined regular arrays of gold nanostructures, which subsequently have been coated with thin films of diamond-like carbon with 25, 55 and 100 nm thickness. Femtosecond laser scanning microscopy enables us to identify enhancement of the second harmonic response of the fibers. This is facilitated by a preservation of the field enhancement effects, which appear on the nanostructures and remain significant on top of the coating layer.

Application of a grating coupler for surface plasmon polariton excitation in a photoemission electron microscopy experiment

Surface plasmon polariton (SPP) excitation at a gold-vacuum interface via 800 nm light pulses mediated by a periodic array of gold ridges is probed at high lateral resolution by means of photoemission electron microscopy (PEEM). We directly monitor and quantify the coupling properties as a function of the number of grating ridges and compare the PEEM results with analytic calculations. An increase in the coupling efficiency of ≈ 3 is observed when increasing the number of ridges from 1 to 6. We observe, however, that a further addition of ridges is rather ineffective. This saturation behavior is assigned to the grazing incidence excitation geometry intrinsic to a conventional PEEM scheme and the limited propagation distance of the SPP modes at the gold-vacuum interface at the used wavelength.