Two-dimensional (2D) materials, such as graphene and single-layer (SL) transition metal dichalcogenides (TMDCs), have attracted a lot of attention due to their fascinating electronic and optical properties. Graphene was the first 2D material that has successfully been exfoliated from bulk graphite in 2004. In graphene, charge carriers interacting with the honeycomb lattice of carbon atoms of graphene to appear as massless Dirac fermions. Massless quasiparticles with linear dispersion are also observed in surface states of 3D topological insulators and quantum Hall edge states. My first project deals with the two-dimensional Hong-Ou-Mandel (HOM) type interference experiment for massless Dirac fermions in graphene and 3D topological insulators. Since massless Dirac fermions exhibit linear dispersion, similar to photons in vacuum, they can be used to observe the HOM interference intensity pattern as a function of the delay time between two massless Dirac fermions. My further projects and the major part of this dissertation deal with single-layer (SL) transition metal dichalcogenides (TMDCs), such as MoS$_2$, WS$_2$, MoSe$_2$ and WSe$_2$, which have recently emerged as a new family of two-dimensional (2D) materials with great interest, not only from the fundamental point of view, but also because of their potential application to ultrathin electronic and optoelectronic devices. In contrast to graphene, SL TMDCs are direct band semiconductors and exhibit large intrinsic spin-orbit coupling (SOC), originating from the d orbitals of transition metal atoms. Wafer-scale production of SL TMDCs is required for industrial applications. It has been shown that artificially grown samples of SL TMDCs through various experimental techniques, such as physical vapor deposition (PVD), chemical vapor deposition (CVD), and molecular beam epitaxy (MBE), are not perfect, instead certain type of imperfections such as point defects are always found to be present in the grown samples. Defects compromise the crystallinity of the sample, which results in reduced carrier mobility and deteriorated optical efficiency. However, defects are not always unwanted; in fact, defects can play an important role in tailoring electronic, optical, and magnetic properties of materials. Using Density functional theory we investigate the impact of point defects on the electronic, optical, and magnetic properties of SL TMDCs. First, we show that certain vacancy defects lead to localized defect states, which in turn give rise to sharp transitions in in-plane and out-of-plane optical susceptibilities of SL TMDCs. Secondly, we show that a naturally occurring antisite defect Mo$_S$ in PVD grown MoS$_2$ is magnetic in nature with a magnetic moment of 2$\mu_B$, and remarkably exhibit an exceptionally large atomic scale magnetic anisotropy energy (MAE) of ~ 500 eV. Both magnetic moment and MAE can be tuned by shifting the position of the Fermi level which can be achieved either by gate voltage or by chemical doping. Thirdly, we argue that the antisite defect Se$_W$ in WSe$_2$ leads to long lived localized excited states, which can explain the observed single quantum emitters in CVD grown WSe$_2$ samples, with potential application to quantum cryptography.
Doctor of Philosophy (Ph.D.)
College of Sciences
Length of Campus-only Access
Doctoral Dissertation (Open Access)
Khan, Mahtab, "Electronic, Optical, and Magnetic Properties of Graphene and Single-Layer Transition Metal Dichalcogenides in the Presence of Defects" (2018). Electronic Theses and Dissertations. 5839.