Chemical Vapor Deposition Grown Pristine and Chemically Doped Monolayer Graphene

Chemical vapor deposition growth has been a popular technique to produce large-area, high-quality monolayer graphene on Cu substrates ever since its first demonstration in 2009. Pristine graphene grown in such a way owns the natures of zero charge carriers and zero band gap. As an analogy to semi-conductor studies, substitutional doping with foreign atoms is a powerful way to tailor the electronic properties of this host materials. Within such a context, this thesis focuses on growing and characterizing both pristine and chemically-doped CVD grown monolayer graphene films at microscopic scales. We first synthesized pristine graphene on Cu single crystals in ultra-high-vacuum and subsequently characterized their properties by scanning tunneling microscopy/spectroscopy (STM/S), to learn the effects of Cu substrate crystallinity on the quality of graphene growth and understand the interactions between graphene films and Cu substrates. In the subsequent chapters, we chemically doped graphene with nitrogen (N) and boron (B) atoms, and characterized their topographic and electronic structures via STM/S. We found that both N and B dopants substitionally dope graphene films, and contribute electron and hole carriers, respectively, into graphene at a rate of approximately 0.5 carrier/dopant. Apart from this, we have made comparisons between N- and B-doped graphene films in aspects of topographic features, dopant distribution and electronic perturbations. In the last part of this thesis, we used Raman spectroscopy mapping to investigate the N dopant distribution within and across structural grains. Future experiments are also brief discussed at the end of the thesis

Electric quadrupole second harmonic generation revealing dual magnetic orders in a magnetic Weyl semimetal

Broken symmetries and electronic topology are nicely manifested together in the second order nonlinear optical responses from topologically nontrivial materials. While second order nonlinear optical effects from the electric dipole (ED) contribution have been extensively explored in polar Weyl semimetals (WSMs) with broken spatial inversion (SI) symmetry, they are rarely studied in centrosymmetric magnetic WSMs with broken time reversal (TR) symmetry due to complete suppression of the ED contribution. Here, we report experimental demonstration of optical second harmonic generation (SHG) in a magnetic WSM Co$_{3}$Sn$_{2}$S$_{2}$ from the electric quadrupole (EQ) contribution. By tracking the temperature dependence of the rotation anisotropy (RA) of SHG, we capture two magnetic phase transitions, with both the SHG intensity increasing and its RA pattern rotating at $T_{C,1}$=175K and $T_{C,2}$=120K subsequently. The fitted critical exponents for the SHG intensity and RA orientation near $T_{C,1}$ and $T_{C,2}$ suggest that the magnetic phase at $T_{C,1}$ is a 3D Ising-type out-of-plane ferromagnetism while the other at $T_{C,2}$ is a 3D XY-type all-in-all-out in-plane antiferromagnetism. Our results show the success of detection and exploration of EQ SHG in a centrosymmetric magnetic WSM, and hence open the pathway towards the future investigation of its tie to the band topology.Comment: 19 pages, 4 figure

Structural investigation of the bilayer iridate Sr_3Ir_2O_7

A complete structural solution of the bilayer iridate compound Sr_3Ir_2O_7 presently remains outstanding. Previously reported structures for this compound vary and all fail to explain weak structural violations observed in neutron scattering measurements as well as the presence of a net ferromagnetic moment in the basal plane. In this paper, we present single crystal neutron diffraction and rotational anisotropy second harmonic generation measurements unveiling a lower, monoclinic symmetry inherent to Sr_3Ir_2O_7. Combined with density functional theory, our measurements identify the correct structural space group as No. 15 (C2/c) and provide clarity regarding the local symmetry of Ir^(4+) cations within this spin-orbit Mott material

Modification of the G-phonon mode of graphene by nitrogen doping

The effect of nitrogen doping on the phonon spectra of graphene is analyzed. In particular, we employ first-principles calculations and scanning Raman analysis to investigate the dependence of phonon frequencies in graphene on the concentration of nitrogen dopants. We demonstrate that the G phonon frequency shows oscillatory behavior as a function of nitrogen concentration. We analyze different mechanisms which could potentially be responsible for this behavior, such as Friedel charge oscillations around the localized nitrogen impurity atom, the bond length change between nitrogen impurity and its nearest neighbor carbon atoms, and the long-range interactions of the nitrogen point defects. We show that the bond length change and the long range interaction of point defects are possible mechanisms responsible for the oscillatory behavior of the G frequency as a function of nitrogen concentration. At the same time, Friedel charge oscillations are unlikely to contribute to this behavior

Modification of the G-phonon mode of graphene by nitrogen doping

The effect of nitrogen doping on the phonon spectra of graphene is analyzed. In particular, we employ first-principles calculations and scanning Raman analysis to investigate the dependence of phonon frequencies in graphene on the concentration of nitrogen dopants. We demonstrate that the G phonon frequency shows oscillatory behavior as a function of nitrogen concentration. We analyze different mechanisms which could potentially be responsible for this behavior, such as Friedel charge oscillations around the localized nitrogen impurity atom, the bond length change between nitrogen impurity and its nearest neighbor carbon atoms, and the long-range interactions of the nitrogen point defects. We show that the bond length change and the long range interaction of point defects are possible mechanisms responsible for the oscillatory behavior of the G frequency as a function of nitrogen concentration. At the same time, Friedel charge oscillations are unlikely to contribute to this behavior