2018, Jia, G., Plentz, J., Gawlik, A., Azar, A.S., Stokkan, G., Syvertsen, M., Carvalho, P.A., Dellith, J., Dellith, A., Andrä, G., Ulyashin, A.

In this study, laser-treated polycrystalline Si (pc-Si) wafers, fabricated by wire sawing of hot-pressed ingots sintered from Si powder, have been investigated. As-cut wafers and those with high-quality thin Si layers deposited on top of them by e-beam have been subjected to laser irradiation to clarify typical trends of structural modifications caused by laser treatments. Moreover, possibility to use laser-treated Si powder-based substrates for fabrication of advanced Si structures has been analysed. It is established that (i) Si powder-based wafers with thicknesses 180 μm can be fully (from the front to back side) or partly (subsurface region) remelted by a diode laser and grain sizes in laser-treated regions can be increased; (ii) a high-quality top layer can be fabricated by crystallization of an additional a-Si layer deposited by e-beam evaporation on top of the pc-Si; and (iii) silicon nanowires can be formed by metal-assisted wet chemical etching (MAWCE) of polished Si powder-based wafers and as-cut wafers irradiated with medium laser power, while a surface texturing on the as-cut pc-Si wafers occur, and no nanowires can form in the region subject to a liquid phase crystallization (LPC) caused by high-power laser treatments.

2018, Trautmann, S., Richard-Lacroix, M., Dathe, A., Schneidewind, H., Dellith, J., Fritzsche, W., Deckert, V.

The optical response of realistic 3D plasmonic substrates composed of randomly shaped particles of different size and interparticle distance distributions in addition to nanometer scale surface roughness is intrinsically challenging to simulate due to computational limitations. Here, we present a Finite Element Method (FEM)-based methodology that bridges in-depth theoretical investigations and experimental optical response of plasmonic substrates composed of such silver nanoparticles. Parametrized scanning electron microscopy (SEM) images of surface enhanced Raman spectroscopy (SERS) active substrate and tip-enhanced Raman spectroscopy (TERS) probes are used to simulate the far-and near-field optical response. Far-field calculations are consistent with experimental dark field spectra and charge distribution images reveal for the first time in arbitrary structures the contributions of interparticle hybridized modes such as sub-radiant and super-radiant modes that also locally organize as basic units for Fano resonances. Near-field simulations expose the spatial position-dependent impact of hybridization on field enhancement. Simulations of representative sections of TERS tips are shown to exhibit the same unexpected coupling modes. Near-field simulations suggest that these modes can contribute up to 50% of the amplitude of the plasmon resonance at the tip apex but, interestingly, have a small effect on its frequency in the visible range. The band position is shown to be extremely sensitive to particle nanoscale roughness, highlighting the necessity to preserve detailed information at both the largest and the smallest scales. To the best of our knowledge, no currently available method enables reaching such a detailed description of large scale realistic 3D plasmonic systems.

2016, Trautmann, S., Aizpurua, J., Götz, I., Undisz, A., Dellith, J., Schneidewind, H., Rettenmayr, M., Deckert, V.

Recent experiments have evidenced sub-nanometer resolution in plasmonic-enhanced probe spectroscopy. Such a high resolution cannot be simply explained using the commonly considered radii of metallic nanoparticles on plasmonic probes. In this contribution the effects of defects as small as a single atom found on spherical plasmonic particles acting as probing tips are investigated in connection with the spatial resolution provided. The presence of abundant edge and corner sites with atomic scale dimensions in crystalline metallic nanoparticles is evident from transmission electron microscopy (TEM) images. Electrodynamic calculations based on the Finite Element Method (FEM) are implemented to reveal the impact of the presence of such atomic features in probing tips on the lateral spatial resolution and field localization. Our analysis is developed for three different configurations, and under resonant and non-resonant illumination conditions, respectively. Based on this analysis, the limits of field enhancement, lateral resolution and field confinement in plasmon-enhanced spectroscopy and microscopy are inferred, reaching values below 1 nanometer for reasonable atomic sizes.