Infrared Spectroscopy of Graphene in Ultrahigh Magnetic Fields
Doctor of Philosophy
Graphene – a two-dimensional honeycomb lattice of sp2-bonded carbon atoms – possesses unusual zero-gap band structure with linear band dispersions, accommodating photon-like, massless electrons that have exhibited a variety of surprising phenomena, primarily in DC transport, in the last several years. In this thesis dissertation, we investigate graphene’s AC or infrared properties in the presence of an ultrahigh magnetic field, produced by a destructive pulsed method. The linear dispersions of graphene lead to unequally spaced Landau levels in a magnetic field, which we probe through cyclotron resonance (CR) spectroscopy in the magnetic quantum limit. Specifically, using magnetic fields up to 170 T and polarized midinfrared radiation with tunable wavelengths from 9.22 to 10.67 μm, we experimentally investigated CR in large-area graphene grown by chemical vapor deposition. Circular-polarization-dependent studies revealed strong p-type doping for as-grown graphene, and the dependence of the CR fields on the radiation wavelength allowed for an accurate determination of the Fermi energy. Upon annealing the sample to remove physisorbed molecules, which shifts the Fermi energy closer to the Dirac point, we made the unusual observation that hole and electron CR emerges in the magnetic quantum limit, even though the sample is still p-type. We theoretically show that this non-intuitive phenomenon is a direct consequence of the unusual Landau level structure of graphene. Namely, if the Fermi energy lies in the n = 0 Landau level, then CR is present for both electron-active and hole-active circular polarizations. Furthermore, if the Fermi level lies in the n = 0 Landau level, the ratio of CR absorption between the electron-active and hole-active peaks allows one to accurately determine the Fermi level and carrier density. Hence, high-field CR studies allow not only for fundamental studies but also for characterization of large-area, low-mobility graphene samples.
Graphene; Ultrahigh magnetic fields; Single-turn coil; Landau levels