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Register a new userRaman Spectroscopy of Graphene under Uniaxial Stress: Phonon Softening and Determination of the Crystallographic Orientation
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We present a systematic study of the Raman spectra of optical phonons in graphene monolayers under tunable uniaxial tensile stress. Both the G and 2D bands exhibit significant red shifts. The G band splits into two distinct sub-bands (G+, G-) because of the strain-induced symmetry breaking. Raman scattering from the G+ and G- bands shows a distinctive polarization dependence that reflects the angle between the axis of the stress and the underlying graphene crystal axes. Polarized Raman spectroscopy therefore constitutes a purely optical method for the determination of the crystallographic orientation of graphene.
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The magneto-phonon resonance or MPR occurs in semiconductor materials when the energy spacing between Landau levels is continuously tuned to cross the energy of an optical phonon mode. MPRs have been largely explored in bulk semiconductors, in two-dimensional systems and in quantum dots. Recently there has been significant interest in the MPR interactions of the Dirac fermion magnetoexcitons in graphene, and a rich splitting and anti-crossing phenomena of the even parity E2g long wavelength optical phonon mode have been theoretically proposed and experimentally observed. The MPR has been found to crucially depend on disorder in the graphene layer. This is a feature that creates new venues for the study of interplays between disorder and interactions in the atomic layers. We review here the fundamentals of MRP in graphene and the experimental Raman scattering works that have led to the observation of these phenomena in graphene and graphite.
Graphene edges are of particular interest, since their chirality determines the electronic properties. Here we present a detailed Raman investigation of graphene flakes with well defined edges oriented at different crystallographic directions. The position, width and intensity of G and D peaks at the edges are studied as a function of the incident light polarization. The D-band is strongest for light polarized parallel to the edge and minimum for perpendicular orientation. Raman mapping shows that the D peak is localized in proximity of the edge. The D to G ratio does not always show a significant dependence on edge orientation. Thus, even though edges can appear macroscopically smooth and oriented at well defined angles, they are not necessarily microscopically ordered.
We derive a general relation between the fine structure splitting (FSS) and the exciton polarization angle of self-assembled quantum dots (QDs) under uniaxial stress. We show that the FSS lower bound under external stress can be predicted by the exciton polarization angle and FSS under zero stress. The critical stress can also be determined by monitoring the change in exciton polarization angle. We confirm the theory by performing atomistic pseudopotential calculations for the InAs/GaAs QDs. The work provides a deep insight into the dots asymmetry and their optical properties, and a useful guide in selecting QDs with smallest FSS which are crucial in entangled photon sources applications.
Microwave measurements have recently been successfully applied to measure ferroelectric materials on the nanoscale, including detection of polarization switching and ferroelectric domain walls. Here we discuss the question whether scanning probe microscopy (SPM) operating at microwave frequency can identify the changes associated with the soft phonon dynamics in a ferroic. The analytical expressions for the electric potential, complex impedance and dielectric losses are derived and analyzed, since these physical quantities are linked to experimentally-measurable properties of the ferroic. As a ferroic we consider virtual or proper ferroelectric with an optic phonon mode that softens at a Curie point. We also consider a decay mechanism linked to the conductance of the ferroic, and thus manifesting itself as the dielectric loss in the material. Our key finding is that the influence of the soft phonon dispersion on the surface potential distribution, complex impedance and dielectric losses are evidently strong in the vicinity (10-30 K) of the Curie temperature. Furthermore, we quantified how the spatial distribution and frequency spectra of the complex impedance and the dielectric losses react on the dynamics of the soft phonons near the Curie point. These results set the stage for characterization of polar phase transitions with nanoscale microwave measurements, providing a complementary approach to well established electromechanical measurements for fundamental understanding of ferroelectric properties as well as their applications in telecommunication and computing.
The equilibrium optical phonons of graphene are well characterized in terms of anharmonicity and electron-phonon interactions, however their non-equilibrium properties in the presence of hot charge carriers are still not fully explored. Here we study the Raman spectrum of graphene under ultrafast laser excitation with 3ps pulses, which trade off between impulsive stimulation and spectral resolution. We localize energy into hot carriers, generating non-equilibrium temperatures in the ~1700-3100K range, far exceeding that of the phonon bath, while simultaneously detecting the Raman response. The linewidth of both G and 2D peaks show an increase as function of the electronic temperature. We explain this as a result of the Dirac cones broadening and electron-phonon scattering in the highly excited transient regime, important for the emerging field of graphene-based photonics and optoelectronics.
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