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search.filters.applied.f.access: openAccess × End date: 2019 × DDC: 540 × DDC: 600 × Publisher: Cambridge : RSC Publ. ×

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    Plasmon response evaluation based on image-derived arbitrary nanostructures
    (Cambridge : RSC Publ., 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.
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    Nanoscale patterning of self-assembled monolayer (SAM)-functionalised substrates with single molecule contact printing
    (Cambridge : RSC Publ., 2017) Sajfutdinow, M.; Uhlig, K.; Prager, A.; Schneider, C.; Abel, B.; Smith, D.M.
    Defined arrangements of individual molecules are covalenty connected ("printed") onto SAM-functionalised gold substrates with nanometer resolution. Substrates were initially pre-functionlised by coating with 3,3′-dithiodipropionic acid (DTPA) to form a self-assembled monolayer (SAM), which was characterised by atomic force microscopy (AFM), contact angle goniometry, cyclic voltammetry and surface plasmon resonance (SPR) spectroscopy. Pre-defined "ink" patterns displayed on DNA origami-based single-use carriers ("stamp") were covalently conjugated to the SAM using 1-ethyl-3-(3-dimethylamino-propyl)carbodiimide (EDC) and N-hydroxy-succinimide (NHS). These anchor points were used to create nanometer-precise single-molecule arrays, here with complementary DNA and streptavidin. Sequential steps of the printing process were evaluated by AFM and SPR spectroscopy. It was shown that 30% of the detected arrangements closely match the expected length distribution of designed patterns, whereas another 40% exhibit error within the range of only 1 streptavidin molecule. SPR results indicate that imposing a defined separation between molecular anchor points within the pattern through this printing process enhances the efficiency for association of specific binding partners for systems with high sterical hindrance. This study expands upon earlier findings where geometrical information was conserved by the application of DNA nanostructures, by establishing a generalisable strategy which is universally applicable to nearly any type of prefunctionalised substrate such as metals, plastics, silicates, ITO or 2D materials.
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    A classical description of subnanometer resolution by atomic features in metallic structures
    (Cambridge : RSC Publ., 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.