Disorder-induced electronic, magnetic, and optoelectronic properties of two-dimensional materials

Technological advancement has been in cadence with material development by improving the purity of single crystals and, at the same time, controlling their imperfections. These capabilities have been especially vital for developing new technolo-gies based on two-dimensional (2D) van der Waals (vdW) materials for future electronic and optoelectronic applications. This is because the inherent properties of 2D vdW materials is highly susceptible to the presence of intrinsic structural defects and ex-trinsic disorders due to large surface-area-to-volume ratio. The successful reduction of these disorders has significantly im-proved material properties and led to the discovery of novel physical phenomena in vdW materials. On the other hand, structural defects – for instance, 0-dimensional point defects – can induce completely new properties that are otherwise absent in the pre-fect lattice. To harness the full potential of vdW materials, it is thus essential to produce high-quality crystals and understand how the disorder affects their material properties, which is the central idea of this dissertation.In this dissertation, we first present the work of high-quality epitaxial growth of NbS2. Based on atmospheric-pressure chemical vapor deposition, we have successfully synthesized the two polymorphs (2H and 3R) of NbS2 with the largest lateral size grown to date. Their distinct superconducting and metallic properties were examined under low-temperature charge transport, respectively. Our finding demonstrates the practical synthesis method for phase-controllable growth of 2D transition metal dichalcogenides and can benefit future studies in mesoscopic devices and large-area applications of 2D superconductors. Secondly, we present the work of discovering defect-induced novel properties in ultrathin layers of PtSe2. Although bulk PtSe2 is non-magnetic, we observe the appearance of magnetism in monolayer and bilayer PtSe2. We were able to measure the magnetoresistance (MR) of mono- and bilayer PtSe2 under perpendicular magnetic fields using proximitized graphene, and found antiferromagnetic and ferromagnetic MR responses for mono- and bilayer, respectively. The appearance of such different magnetic states is theoretically explained by the first-principle density functional theory calculation, suggesting the origin of induced-magnetic moments from intrinsic Pt vacancies for both layers. Moreover, we also found that structural disorder in PtSe2 can induce bulk photovoltaic effect (BPVE). The second-order optical nonlinear effects, such as BPVE, require broken structural inversion symmetry and crystal symmetry can be reduced by the presence of structural defects. The broken local inversion symmetry from structural disorder in centrosymmetric PtSe2 is manifested by the generation of zero-biased photo-current under homogenous illumination. We observe linear and circular polarization-dependent photocurrents in defective PtSe2, which is largely absent in the pristine crystal. Our findings in PtSe2 emphasize the importance of the structural disorder for generating completely new properties and stress the need for defect-engineering for realizing the practical use of PtSe2 in spintronic and photovoltaic applications.