In this report, we present Raman spectroscopy investigation of the thermal stability and dynamics of graphene edges. It was found that graphene edges (both armchair and zigzag) are not stable and undergo modifications even at temperature as low as 200°C. Based on polarized Raman results, we provide possible structural models on how graphene edges change during annealing. The zigzag edges rearrange and form armchair segments that are \pm30° relative to the edge direction, while armchair edges are dominated by armchair segments even at annealing temperature as high as 500°C. The modifications of edge structures by thermal annealing (zigzag segments rearrange in form of armchair segments) provide a flexible way to control the electronic properties of graphene and graphene nanostructures.
The unique properties of graphene offer immense opportunities for applications to many scientific fields, as well as societal needs, beyond our present imagination. One of the important features of graphene is the relatively simple tunability of its electronic structure, an asset which extends the usability of graphene even further beyond present experience. A direct injection of charge carriers into the conduction or valence bands, i.e., doping, represents a viable way of shifting the Fermi level. In particular, the electrochemical doping should be the method of choice, when higher doping lev…
Graphene has extraordinary mechanical and electronic properties, making it a promising material for membrane based nanoelectromechanical systems (NEMS). Here, chemical-vapor-deposited graphene is transferred onto target substrates to suspend it over cavities and trenches for pressure-sensor applications. The development of such devices requires suitable metrology methods, i.e., large-scale characterization techniques, to confirm and analyze successful graphene transfer with intact suspended graphene membranes. We propose fast and noninvasive Raman spectroscopy mapping to distinguish between fr…
We report a Raman spectroscopy study of graphene field-effect transistors (GFET) with a controlled amount of defects introduced in graphene by exposure to electron-beam irradiation. Raman spectra are taken at T = 8 K over a range of back gate voltages (Vg) for various irradiation dosages (Re). We study effects in the Raman spectra due to Vg-induced doping and artificially created disorder at various Re. With moderate disorder (irradiation), the Raman G peak with respect to the graphene carrier density (nFE) exhibits a minimum in peak frequency and a maximum in peak width near the charge- neutr…
We present an analysis of deep-UV Raman measurements of graphite, graphene and carbon nanotubes. For excitation energies above the strong optical absorption peak at the $M$ point in the Brillouin zone ($\approx 4.7\,\text{eV}$), we partially suppress double-resonant scattering processes and observe the two-phonon density of states of carbon nanomaterials. The measured peaks are assigned to contributions from LO, TO, and LA phonon branches, supported by calculations of the phonon dispersion. Moreover, we gain access to the infrared-active $E_{1u}$ mode in graphite. By lowering the excitation en…
We present an \textit{ab initio} study based on density-functional theory of first- and second-order Raman spectra of graphene-based materials with different stacking arrangements and numbers of layers. Going from monolayer and bilayer graphene to periodic graphitic structures, we investigate the behavior of the first-order G-band and of the second-order 2D-band excited by the same set of photon energies. The former turns out to be very similar in all considered graphene-based materials, while in the latter we find the signatures of individual structures. With a systematic analysis of the seco…
Comment on "Raman spectra of misoriented bilayer graphene"
在最近的论文[Phys.Rev.B78，113407（2008）]中，Poncharal等人研究了取向错误的双层石墨烯的拉曼光谱。他们发现，相对于单层石墨烯，错位石墨烯的2D带的蓝移显示出对激发激光能量的强烈依赖性。蓝移随激发能的降低而增加。这一发现与我们对折叠/错误取向的石墨烯的费米速度降低的解释相矛盾[Ni et al.Phys.Rev.B77，235403（2008）]。在这篇评论中，我们提出了更多的实验结果，从我们的小组以及从其他人表明，蓝移确实只是弱依赖于激发能。因此，我们认为，我们的解释的二维蓝移的折叠石墨烯由于费米速度的降低仍然是有效的。
As the synthesis of graphene on copper became one of the primary preparation methods for both fundamental research and industrial application, Raman spectra of graphene/Cu systems need to be quantitatively understood regarding how their interactions affect the electronic structure of graphene. Using multi-wavelength Raman spectroscopy, we investigated three types of graphene bound on Cu: graphene grown on Cu foils and Cu film/SiO2, and Cu-evaporated exfoliated graphene. 2D peak frequencies of the first two samples were ~17 cm-1 higher than expected for 1.96 eV excitation even when the effect o…
Raman spectroscopy plays a key role in studies of graphene and related carbon systems. Graphene is perhaps the most promising material of recent times for many novel applications, including electronics. In this paper, the traditional and well established Kramers-Heisenberg-Dirac (KHD) Raman scattering theory (1925-1927) is extended to crystalline graphene for the first time. It demands different phonon production mechanisms and phonon energies than does the popular "double resonance" Raman scattering model. The latter has never been compared to KHD. Within KHD, phonons are produced instantly a…
Raman spectroscopy is a powerful tool for characterizing the local properties of graphene. Here, we introduce a method for evaluating unknown strain configurations and simultaneous doping. It relies on separating the effects of hydrostatic strain (peak shift) and shear strain (peak splitting) on the Raman spectrum of graphene. The peak shifts from hydrostatic strain and doping are separated with a correlation analysis of the 2D and G frequencies. This enables us to obtain the local hydrostatic strain, shear strain and doping without any assumption on the strain configuration prior to the analy…
Accurate and simple local strain assessment in graphene is one of the crucial tasks in device characterization. Raman spectroscopy is often used for that purpose through monitoring of the G and 2D modes. However, the shifts of those two bands might be biased, especially under uniaxial strain, by the effects of charge-transfer doping. Therefore, it is extremely desirable to use another Raman band, less affected by doping, but with a defined and measurable behavior under strain. The Raman 2D' mode is in this sense the ideal feature for the evaluation of strain levels in stretched graphene monola…
Graphite intercalation compounds (GICs) with the geometrical anisotropy and strong electron-phonon coupling are in full swing and have shown their great potential for applications in nanodevices. I selected representative three elements in actinide group with valence electron arrangement: Thorium (Th) ([Rn]6d27s2), Uranium (U) ([Rn]5f36d17s2), Plutonium (Pu) ([Rn]5f67s2). I calculated their phonon spectra and demonstrated the atomic-scale microstructure identification of actinide graphite intercalation compounds by angle-resolved polarized Raman spectroscopy.
We report the growth of thickness-controlled rotationally faulted multilayer graphene (rf-MLG) on Ni foils by low-pressure chemical vapor deposition and their characterization by micro-Raman spectroscopy. The surface morphology and thickness were investigated by scanning electron microscope, X-ray diffraction, and transmittance measurements. These results have revealed that the thickness of rf-MLG can be effectively controlled by the thickness of the Ni foil rather than the flow rate of CH$_4$, H$_2$, Ar. In the Raman spectroscopy measurements, we observed most Raman peaks of the graphitic mat…
The polarized Raman spectroscopy is capable of giving confirmation regarding the crystalline phase as well as the crystallographic orientation of the sample. In this context, apart from crystallographic x-ray and electron diffraction tools, polarized Raman spectroscopy and corresponding spectral imaging can be a promising crystallographic tool for determining both crystalline phase and orientation. Sub-micron sized hexagonal AlGaN crystallites are grown by a simple atmospheric pressure chemical vapor deposition technique using the self catalytic vapor-solid process under N-rich condition. The …
We investigated 10 to 200 nm thick black phosphorus flakes on SiO2/Si and polyimide substrates by Angle-resolved Polarized Raman spectra (ARPRS) using 442 nm excitation wavelength. The results revealed that ARPRS with 442 nm excitation can provide unambiguous, convenient, non-destructive and fast determination of BP's crystallographic orientation. The substrate and thickness dependencies of Raman spectra and Raman tensor elements were studied. These dependencies were shown to be influenced by Raman excitation laser heating effect. By comparing with in-situ Raman measurements at elevated temper…
In the last decade, hybrid organic-inorganic halide perovskites have emerged as a new type of semiconductor for photovoltaics and other optoelectronic applications. Unlike standard, tetrahedrally bonded semiconductors (e.g. Si and GaAs), the ionic thermal fluctuations in the halide perovskites (i.e. structural dynamics) are strongly coupled to the electronic dynamics. Therefore, it is crucial to obtain accurate and detailed knowledge about the nature of atomic motions within the crystal. This has proved to be challenging due to low thermal stability and the complex, temperature dependent struc…
We describe Raman spectroscopy based method of measuring thermal conductivity of thin films, and review significant results achieved with this technique pertinent to graphene and other two-dimensional materials. The optothermal Raman method was instrumental for the discovery of unique heat conduction properties of graphene. In this method, Raman spectroscopy is used to determine the local temperature of the sample while the excitation laser is utilized as a heat source. The success of Raman spectroscopy in investigating thermal conductivity of suspended graphene and graphene-based thin films m…
We review the different results obtained in the last decade in the field of Raman scattering of graphene based systems, with an applied magnetic field. Electronic properties of graphene based systems with an applied magnetic field will first be described. The phonon response in magnetic field, the magneto-phono resonance, will then be introduced and described in different systems, including graphene, multilayer graphene and bulk graphite. Electronic Raman scattering is then be discussed in the context of Landau level spectroscopy, of electron phonon interaction and of electron-electron interac…
We synthesized three-dimensional nanoporous graphene films by a chemical vapor deposition method with nanoporous copper as a catalytic substrate. The resulting nanoporous graphene has the same average pore size as the underlying copper substrate. Our surface-enhanced Raman scattering (SERS) investigation indicates that the nanoporosity of graphene significantly improves the SERS efficiency of graphene as a substrate as compared to planar graphene substrates.
Graphene layers placed on SrTiO3 single-crystal substrates were investigated using temperature-dependent confocal Raman spectroscopy. This approach successfully resolved distinct Raman modes of graphene that are often untraceable in conventional measurements due to the strong Raman scattering background of SrTiO3. Information on defects and strain states was obtained for a few graphene/SrTiO3 samples that were synthesized by different techniques. This confocal Raman spectroscopic approach can shed light on the investigation of not only this graphene/SrTiO3 system but also various two-dimension…
Raman spectroscopy of graphene on different substrates and influence of defects
我们展示了拉曼光谱随不同衬底上石墨烯层数的演变，SiO $_{2}$ /Si和导电氧化铟锡（ITO）板。对于相同层数的石墨烯，G模峰位以及G带和2D带的强度比取决于样品的制备。2D拉曼谱带在单层和双层石墨烯中具有特征线形状，捕获了它们电子结构的差异。缺陷对单层石墨烯的G带峰位置具有显著影响：取决于D拉曼带的强度，频率显示出高达12 cm $^{-1}$的蓝移，这是缺陷密度的标志。最令人惊讶的是，导电ITO板上的石墨烯的拉曼光谱显示出$\sim$ 6 cm $^{-1}$的G模式频率和$\sim$ 20 cm $^{-1}$的2D带频率的降低。G和2D带的这种红移是在单层石墨烯中首次观察到的。
