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Register a new userSurface-enhanced Raman scattering of graphene caused by self-induced nanogating by GaN nanowire array
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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.
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We present detailed Raman studies of graphene deposited on gallium nitride nanowires with different variations in height. Our results show that different density and height of nanowires being in contact with graphene impact graphene properties like roughness, strain and carrier concentration as well as density and type of induced defects. Detailed analysis of Raman spectra of graphene deposited on different nanowire substrates shows that bigger differences in nanowires height increase graphene strain, while higher number of nanowires in contact with graphene locally reduce the strain. Moreover, the value of graphene carrier concentration is found to be correlated with the density of nanowires in contact with graphene. Analysis of intensity ratios of Raman G, D and D bands enable to trace how nanowire substrate impacts the defect concentration and type. The lowest concentration of defects is observed for graphene deposited on nanowires of the lowest density. Contact between graphene and densely arranged nanowires leads to a large density of vacancies. On the other hand, grain boundaries are the main type of defects in graphene on rarely distributed nanowires. Our results also show modification of graphene carrier concentration and strain by different types of defects present in graphene.
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.
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.
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.
Umklapp processes play a fundamental role as the only intrinsic mechanism that allows electrons to transfer momentum to the crystal lattice and, therefore, provide a finite electrical resistance in pure metals. However, umklapp scattering has proven to be elusive in experiment as it is easily obscured by other dissipation mechanisms. Here we show that electron-electron umklapp scattering dominates the transport properties of graphene-on-boron-nitride superlattices over a wide range of temperatures and carrier densities. The umklapp processes cause giant excess resistivity that rapidly increases with increasing the superlattice period and are responsible for deterioration of the room-temperature mobility by more than an order of magnitude as compared to standard, non-superlattice graphene devices. The umklapp scattering exhibits a quadratic temperature dependence accompanied by a pronounced electron-hole asymmetry with the effect being much stronger for holes rather than electrons. Aside from fundamental interest, our results have direct implications for design of possible electronic devices based on heterostructures featuring superlattices.
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