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Register a new userProbing electronic lifetimes and phonon anharmonicities in high-quality chemical vapor deposited graphene by magneto-Raman spectroscopy
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We present a magneto-Raman study on high-quality single-layer graphene grown by chemical vapor deposition (CVD) that is fully encapsulated in hexagonal boron nitride by a dry transfer technique. By analyzing the Raman D, G, and 2D peaks, we find that the structural quality of the samples is comparable to state-of-the-art exfoliated graphene flakes. From B field dependent Raman measurements, we extract the broadening and associated lifetime of the G peak due to anharmonic effects. Furthermore, we determine the decay width and lifetime of Landau level (LL) transitions from magneto-phonon resonances as a function of laser power. At low laser power, we find a minimal decay width of 140 1/cm highlighting the high electronic quality of the CVD-grown graphene. At higher laser power, we observe an increase of the LL decay width leading to a saturation with the corresponding lifetime saturating at a minimal value of 18 fs.
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Chemical vapor deposited (CVD) graphene is often presented as a scalable solution to graphene device fabrication, but to date such graphene has exhibited lower mobility than that produced by exfoliation. Using a boron nitride underlayer, we achieve mobilities as high as 37,000 cm^2/Vs, an order of magnitude higher than commonly reported for CVD graphene and better than most exfoliated graphene. This result demonstrates that the barrier to scalable, high mobility CVD graphene is not the growth technique but rather the choice of a substrate that minimizes carrier scattering.
We have investigated the effects of ozone treatment on graphene by Raman scattering. Sequential ozone short-exposure cycles resulted in increasing the $p$ doping levels as inferred from the blue shift of the 2$D$ and $G$ peak frequencies, without introducing significant disorder. The two-phonon 2$D$ and 2$D$ Raman peak intensities show a significant decrease, while, on the contrary, the one-phonon G Raman peak intensity remains constant for the whole exposure process. The former reflects the dynamics of the photoexcited electrons (holes) and, specifically, the increase of the electron-electron scattering rate with doping. From the ratio of 2$D$ to 2$D$ intensities, which remains constant with doping, we could extract the ratio of electron-phonon coupling parameters. This ratio is found independent on the number of layers up to ten layers. Moreover, the rate of decrease of 2$D$ and 2$D$ intensities with doping was found to slowdown inversely proportional to the number of graphene layers, revealing the increase of the electron-electron collision probability.
Magneto-Raman scattering experiments from the surface of graphite reveal novel features associated to purely electronic excitations which are observed in addition to phonon-mediated resonances. Graphene-like and graphite domains are identified through experiments with $sim 1mu m$ spatial resolution performed in magnetic fields up to 32T. Polarization resolved measurements emphasize the characteristic selection rules for electronic transitions in graphene. Graphene on graphite displays the unexpected hybridization between optical phonon and symmetric across the Dirac point inter Landau level transitions. The results open new experimental possibilities - to use light scattering methods in studies of graphene under quantum Hall effect conditions.
Integration of graphene with Si microelectronics is very appealing by offering potentially a broad range of new functionalities. New materials to be integrated with Si platform must conform to stringent purity standards. Here, we investigate graphene layers grown on copper foils by chemical vapor deposition and transferred to silicon wafers by wet etch and electrochemical delamination methods with respect to residual sub-monolayer metallic contaminations. Regardless of the transfer method and associated cleaning scheme, time-of-flight secondary ion mass spectrometry and total reflection x-ray fluorescence measurements indicate that the graphene sheets are contaminated with residual metals (copper, iron) with a concentration exceeding 10$^{13}$ atoms/cm$^{2}$. These metal impurities appear to be partly mobile upon thermal treatment as shown by depth profiling and reduction of the minority charge carrier diffusion length in the silicon substrate. As residual metallic impurities can significantly alter electronic and electrochemical properties of graphene and can severely impede the process of integration with silicon microelectronics these results reveal that further progress in synthesis, handling, and cleaning of graphene is required on the way to its advanced electronic and optoelectronic applications.
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.
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