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Register a new userEffects of Quantum Tunneling in Metal Nano-gap on Surface-Enhanced Raman Scattering
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The quantum tunneling effects between two metallic plates are studied using the time dependent density functional theory. Results show that the tunneling is mainly dependent on the separation and the initial local field of the interstice between plates. The smaller separation and larger local field, the easier the electrons tunnels through the interstice. Our numerical calculation shows that when the separation is smaller than 0.6 nm the quantum tunneling dramatically reduce the enhancing ability of interstice between nanoparticles.
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Surface-enhanced Raman spectroscopy is a powerful and versatile sensing method with a detection limit down to the single molecule level. In this article, we demonstrate how topology optimization (TopOpt) can be used for designing surface enhanced Raman scattering (SERS) substrates adhering to realistic fabrication constraints. As an example, we experimentally demonstrated a SERS enhancement factor of 5*10e4 for the 604 cm-1 Raman line of rhodamine 6G using metal nanostructures with a critical dimension of 20 nm. We then show that, by relaxing the fabrication constraints, TopOpt may be used to design SERS substrates with orders of magnitude larger enhancement factor. The results validate topology optimization as an effective method for engineering nanostructures with optimal performance and fabrication tolerance.
The surface-enhanced Raman scattering in graphene deposited on AlxGa1-xN/GaN axial heterostructure nanowires was investigated. The intensity of graphene Raman spectra was found not to be correlated with aluminium content. Analysis of graphene Raman bands parameters, KPFM and electroreflectance showed a screening of polarization charges. Theoretical calculations showed that plasmon resonance in graphene is far beyond the Raman spectral range. This excludes the presence of an electromagnetic mechanism of SERS and therefore suggests the chemical mechanism of enhancement.
The influence of GaN nanowires on the optical and electrical properties of graphene deposited on them was studied using Raman spectroscopy and microwave induced electron transport method. It was found that interaction with the nanowires induces spectral changes as well as large enhancement of Raman scattering intensity. Surprisingly, the smallest enhancement (about 30-fold) was observed for the defect induced D process and the highest intensity increase (over 50-fold) was found for the 2D transition. The observed energy shifts of the G and 2D bands allowed to determine carrier concentration fluctuations induced by GaN nanowires. Comparison of Raman scattering spatial intensity maps and the images obtained using scanning electron microscope led to conclusion that vertically aligned GaN nanowires induce a homogenous strain, substantial spatial modulation of carrier concentration in graphene and unexpected homogenous distribution of defects created by interaction with nanowires. The analysis of the D and D peak intensity ratio showed that interaction with nanowires also changes the probability of scattering on different types of defects. The Raman studies were correlated with weak localization effect measured using microwave induced contactless electron transport. Temperature dependence of weak localization signal showed electron-electron scattering as a main decoherence mechanism with additional, temperature independent scattering reducing coherence length. We attributed it to the interaction of electrons in graphene with charges present on the top of nanowires due to spontaneous and piezoelectric polarization of GaN. Thus, nanowires act as antennas and generate enhanced near field which can explain the observed large enhancement of Raman scattering intensity.
A constant height of gallium nitride (GaN) nanowires with graphene deposited on them is shown to have a strong enhancement of Raman scattering, whilst variable height nanowires fail to give such an enhancement. Scanning electron microscopy reveals a smooth graphene surface which is present when the GaN nanowires are uniform, whereas graphene on nanowires with substantial height differences is observed to be pierced and stretched by the uppermost nanowires. The energy shifts of the characteristic Raman bands confirms that these differences in the nanowire height has a significant impact on the local graphene strain and the carrier concentration. The images obtained by Kelvin probe force microscopy show clearly that the carrier concentration in graphene is modulated by the nanowire substrate and dependent on the nanowire density. Therefore, the observed surface enhanced Raman scattering for graphene deposited on GaN nanowires of comparable height is triggered by self-induced nano-gating to the graphene. However, no clear correlation of the enhancement with the strain or the carrier concentration of graphene was discovered.
Single-molecule detection with chemical specificity is a powerful and much desired tool for biology, chemistry, physics, and sensing technologies. Surface-enhanced spectroscopies enable single molecule studies, yet reliable substrates of adequate sensitivity are in short supply. We present a simple, scaleable substrate for surface-enhanced Raman spectroscopy (SERS) incorporating nanometer-scale electromigrated gaps between extended electrodes. Molecules in the nanogap active regions exhibit hallmarks of very high Raman sensitivity, including blinking and spectral diffusion. Electrodynamic simulations show plasmonic focusing, giving electromagnetic enhancements approaching those needed for single-molecule SERS.
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