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Register a new userInfluence of ageing on Raman spectra and the conductivity of monolayer graphene samples irradiated by heavy and light ions
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The influence of long-term ageing (about one year) on the Raman scattering (RS) spectra and the temperature dependence of conductivity has been studied in two series of monolayer graphene samples irradiated by different doses of C$^{+}$ and Xe$^{+}$ ions. It is shown that the main result of ageing consists of changes in the intensity and position of D- and G- and 2D-lines in RS spectra and in an increase of the conductivity. The observed effects are explained in terms of an increase of the radius of the textquotedblleft activatedtextquotedblright{} area around structural defects.
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The Raman scattering spectra (RS) of two series of monolayer graphene samples irradiated with various doses of C$^{+}$ and Xe$^{+}$ ions were measured after annealing in high vacuum, and in forming gas (95%Ar+5%H$_{2}$). It was found that these methods of annealing have dramatically different influence on the RS lines. Annealing in vacuum below 500$^{circ}$C leads to significant decrease of both D-line, associated with defects, and 2D-line, associated with the intact lattice structure, which can be explained by annealing-induced enhanced doping. Further annealing in vacuum up to 1000$^{circ}$C leads to significant increase of 2D-line together with continuous decrease of D-line, which gives evidence of partial removal of defects and recovery of the damaged lattice. Annealing in forming gas is less effective in this sense. The blue shift of all lines is observed after annealing. It is shown that below 500$^{circ}$C, the unintentional doping is the main mechanism of shift, while at higher annealing temperatures, the lattice strain dominates due to mismatch of the thermal expansion coefficient of graphene and the SiO$_{2}$ substrate. Inhomogeneous distribution of stress and doping across the samples leads to the correlated variation of the amplitude and the peak position of RS lines.
Broadening of the Raman scattering (RS) spectra was studied in monolayer graphene samples irradiated with various dose of ions followed by annealing of radiation damage at different temperatures. It is shown that the width {Gamma} (full width at half maximum, FWHM) of three main RS lines (G-, D-, and 2D) increases linearly with increase of the density of irradiation-induced point defects N d as {Delta}{Gamma} = m N d . The slope m of the linear dependencies is the same for one-phonon emitting G-line and D-line, and almost double for two-phonon emitting 2D-line. It is also shown that the width of D-line {Gamma} D for all samples is larger than one half of the width of 2D-line {Gamma} 2D , which shows that in the case of D-line, elastic electron scattering on point defects leads to an additional decreasing the lifetime of the emitted phonon. Theoretical model of the width of D-line in disordered graphene is developed which explains the experimental observations and allows to determine the numerical coefficient in the in-plane transverse optic phonon dispersion in graphene.
Transport properties of irradiated graphene (electrical conductivity and mobility) are numerically investigated using the real-space Kubo formalism. A micrometer-sized system consisting of millions of atoms with nanopores of various sizes and concentrations is described. Electrical conductivity and mobility as a function of carrier (hole) density are calculated to provide possible comparisons with experiments.
Magnetoresistance (MR) of ion irradiated monolayer graphene samples with variable-range hopping (VRH) mechanism of conductivity was measured at temperatures down to $T = 1.8$ K in magnetic fields up to $B = 8$ T. It was observed that in perpendicular magnetic fields, hopping resistivity $R$ decreases, which corresponds to negative MR (NMR), while parallel magnetic field results in positive MR (PMR) at low temperatures. NMR is explained on the basis of the orbital model in which perpendicular magnetic field suppresses the destructive interference of many paths through the intermediate sites in the total probability of the long-distance tunneling in the VRH regime. At low fields, a quadratic dependence ($|Delta R/R|sim B^2$) of NMR is observed, while at $B > B^*$, the quadratic dependence is replaced by the linear one. It was found that all NMR curves for different samples and different temperatures could be merged into common dependence when plotted as a function of $B/B^*$. It is shown that $B^*sim T^{1/2}$ in agreement with predictions of the orbital model. The obtained values of $B^*$ allowed also to estimate the localization radius $xi$ of charge carriers for samples with different degree of disorder. PMR in parallel magnetic fields is explained by suppression of hopping transitions via double occupied states due to alignment of electron spins.
We show the evolution of Raman spectra with number of graphene layers on different substrates, SiO$_{2}$/Si and conducting indium tin oxide (ITO) plate. The G mode peak position and the intensity ratio of G and 2D bands depend on the preparation of sample for the same number of graphene layers. The 2D Raman band has characteristic line shapes in single and bilayer graphene, capturing the differences in their electronic structure. The defects have a significant influence on the G band peak position for the single layer graphene: the frequency shows a blue shift upto 12 cm$^{-1}$ depending on the intensity of the D Raman band, which is a marker of the defect density. Most surprisingly, Raman spectra of graphene on the conducting ITO plates show a lowering of the G mode frequency by $sim$ 6 cm$^{-1}$ and the 2D band frequency by $sim$ 20 cm$^{-1}$. This red-shift of the G and 2D bands is observed for the first time in single layer graphene.
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