Magnetotransport Studies of Correlated Electronic Phases in Van der Waals Materials

One of the fastest growing fields in condensed matter physics is that of two-dimensional materials; compounds that promise to revolutionize nanotechnology due to the ability to easily isolate clean atomically thin sheets of conducting material for use in atomic-scale circuits. Since the initial demonstration of the electric-field effect in nanocircuits fabricated from mechanically exfoliated graphene, the number of available compounds that can be isolated and used in atomically thin circuits has exponentially grown to include diverse electrical properties from metals and insulators to superconductors and magnets. The bulk compounds from which flakes are isolated are known as van der Waals materials named for their intrinsic structural anisotropy resulting in weak van der Waals chemical bonds in one dimension. Since this field is relatively young, there are a multitude of branching opportunities for experimental advancement. In this work, we begin by addressing a significant technical challenge within the two-dimensional community; contacting and measuring air-sensitive two-dimensional materials. We developed a novel technique for embedding metal electrodes in atomically thin insulating flakes used to simultaneously contact and preserve a wide-array of air-sensitive two-dimensional materials. Using this technique, we proceed to explore the properties of a diverse set of van der Waals compounds in both three dimensions and two dimensions. We investigate the nature of superconductivity in the two-dimensional limit by quantifying the fragility of the superconducting state in a single atomic sheet of NbSe2. In combination with theoretical time-dependent Ginzburg-Landau simulations, we show that the dissipation in two-dimensional NbSe2 can be accurately described by vortex dynamics, including the poorly understood low-temperature metallic-like state. We examine how superconductors proximitize with normal metals through measurements on atomic-scale normal metal/insulator/superconductor tunnel junctions fabricated from van der Waals materials, demonstrating agreement with Blonder- Tinkham-Klapwijk theory. In addition, in junctions fabricated from graphene and NbN, a high-critical- field superconductor, we gain an understanding of Andreev processes in graphene under large magnetic fields. Finally, we provide a detailed characterization Re6Se8Cl2 and CrSBr, two new van der Waals compounds. In Re6Se8Cl2, we develop a novel strategy for doping in van der Waals compounds with labile ligands, demonstrating a semiconducting to superconducting transition upon electron doping. In CrSBr, we discover a well-developed semiconducting gap along with strong coupling between magnetic order and transport properties, unique among van der Waals magnets. Further, we find the semiconducting and magnetic properties persist down to 2 layers of CrSBr, with the observation of air-stability, establishing it as a promising material platform for increasing the applicability of van der Waals magnets