Van der Waals (vdW) magnets provide an exciting opportunity for exploring two-dimensional (2D) magnetism for next generation scientific and technological advances. While previously realized in 3D ultrathin films where the magnetism is stabilized via substrate-assisted magnetic anisotropy, recent reports have shown intrinsic ferromagnetism at low temperatures (< 60 K) in isolated µm-sized flakes mechanically exfoliated from a bulk single-crystal down to a single-atomic layer. This opens up the possibility to truly study magnetism in free-standing 2D layers without direct effects from the underlying substrate and being intrinsically susceptible to surface effects such as atomic adsorbates, electrostatic gating, and proximity-induced phenomena. This dissertation examines the molecular beam epitaxy (MBE) growth and characterization of new 2D magnets, monolayers of MnSe2 and VSe2, that show ferromagnetic ordering above room temperature. Growth on different substrates and varying the substrate temperature during growth affects the growth mode and morphology of the deposited 2D magnet and also affects the measured magnetization. Direct atomic and magnetic imaging via scanning transmission electron microscopy (STEM) and scanning tunneling microscopy (STM) show stable 2D magnetic layers.
Due to the lack of dangling bonds at the surface of these 2D magnets, applying external epitaxial strain is a challenge. Later in this dissertation, the magnetic, electronic, and structural properties of vdW-layered, Fe-deficient Fe3−xGeTe2 are systematically investigated by
he application of high pressure. Fe3GeTe2 is of particular interest due to its high Curie temperature, Tc, strong perpendicular magnetic anisotropy, and tunable magnetic properties depending on the concentration of Fe and its thickness. Electrical and magneto-transport measurements show a suppression in Tc with an increasing pressure up to 20 GPa. The decrease in Tc is due to the lattice shrinkage from pressurization which leads to a weakening of the exchange interaction. These observations showcase the tunability in vdW magnets via pressure which can complement other external stimuli such as chemical doping, making them candidates for future spintronic, electronic and photonic devices.
