This thesis explores an amazing family of oxide compounds - the nickelates - known for their
metal-to-insulator transition and in the case of LaNiO3 to be a possible building block for
designing a synthetic high Tc superconductor. Competition between various fascinating phases
makes these materials very sensitive to external parameters and it is thus possible to
dramatically tune their properties. This work on ultrathin LaNiO3 and the solid solution
Nd1-xLaxNiO3 has important implications for the search for superconductivity in this class of
materials.