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We use mono-crystalline gold platelets with ultra-smooth surfaces and superior plasmonic properties to investigate the formation of interference patterns caused by surface plasmon polaritons (SPPs) with scattering-type scanning near-field microscopy (s-SNOM) at 521~nm and 633~nm. By applying a Fourier analysis approach, we can identify and separate several signal channels related to SPPs launched and scattered by the AFM tip and the edges of the platelet. Especially at the excitation wavelength of 633~nm, we can isolate a region in the center of the platelets where we find only contributions of SPPs which are launched by the tip and reflected at the edges. These signatures are used to determine the SPP wavelength of $\lambda_{SPP}=606$ nm in good agreement with theoretical predictions. Furthermore, we were still able to measure SPP signals after 20~$\upmu$m propagation, which demonstrates impressively the superior plasmonic quality of these mono-crystalline gold platelets., Comment: Main 20 pages, 8 figures, Supplemental Information 5 pages, 3 figures

Gold nanostructures have important applications in nanoelectronics, nano-optics as well as in precision metrology due to their intriguing opto-electronic properties. These properties are governed by the bulk band structure but to some extend are tunable via geometrical resonances. Here we show that the band structure of gold itself exhibits significant size-dependent changes already for mesoscopic critical dimensions below 30 nm. To suppress the effects of geometrical resonances and grain boundaries, we prepared atomically flat ultrathin films of various thicknesses by utilizing large chemically grown single-crystalline gold platelets. We experimentally probe thickness-dependent changes of the band structure by means of two-photon photoluminescence and observe a surprising 100-fold increase of the nonlinear signal when the gold film thickness is reduced below 30 nm allowing us to optically resolve single-unit-cell steps. The effect is well explained by density functional calculations of the thickness-dependent 2D band structure of gold.

The photon spin is an important resource for quantum information processing as is the electron spin in spintronics. However, for subwavelength confined optical excitations, polarization as a global property of a mode cannot be defined. Here, we show that any polarization state of a plane-wave photon can reversibly be mapped to a pseudo-spin embodied by the two fundamental modes of a subwavelength plasmonic two-wire transmission line. We design a device in which this pseudo-spin evolves in a well-defined fashion throughout the device reminiscent of the evolution of photon polarization in a birefringent medium and the behaviour of electron spins in the channel of a spin field-effect transistor. The significance of this pseudo-spin is enriched by the fact that it is subject to spin-orbit locking. Combined with optically active materials to exert external control over the pseudo-spin precession, our findings could enable spin-optical transistors, i.e. the routing and processing of quantum information with light on a subwavelength scale., Comment: 21 pages, 10 figures

Exact quantitative understanding of plasmon propagation along nanowires is mandatory for designing and creating functional devices. Here we investigate plasmon transmission through top-down fabricated monocrystalline gold nanowires on a glass substrate. We show that the transmission through finite-length nanowires can be described by Fabry-P\'{e}rot oscillations that beat with free-space propagating light launched at the incoupling end. Using an extended Fabry-P\'{e}rot model, experimental and simulated length dependent transmission signals agree quantitatively with a fully analytical model., Comment: 5 pages, 4 figures

Chemically synthesized single-crystalline gold microplates have been attracting increasing interests because of their potential as high-quality gold films for nanotechnology. We present the growth of tens of nanometer thick and tens of micrometer large single-crystalline gold plates directly on solid substrates by solution-phase synthesis. Compared to microplates deposited on substrates from dispersion phase, substrate-grown plates exhibit significantly higher quality by avoiding severe small-particle contamination and aggregation. Substrate-grown gold plates also open new perspec-tives to study the growth mechanism via intermittent growth and observation cycles of a large number of individual plates. Growth models are proposed to interpret the evolution of thickness, area and shape of plates. It is found that the plate surface remains smooth after regrowth, implying the application of regrowth for producing giant plates as well as unique single-crystalline nano-structures.

We experimentally demonstrate synthesis and in-situ analysis of multimode plasmonic excitations in two-wire transmission lines supporting a symmetric and an antisymmetric eigenmode. To this end we irradiate an incoupling antenna with a diffraction-limited excitation spot exploiting a polarization- and position-dependent excitation efficiency. Modal analysis is performed by recording the far-field emission of two mode-specific spatially separated emission spots at the far end of the transmission line. To illustrate the power of the approach we selectively determine the group velocities of symmetric and antisymmetric contributions of a multimode ultrafast plasmon pulse.