The layered honeycomb lattice iridate Na2IrO3 is a novel candidate material for either a topological insulator or spin liquid. These states of matter are one possible starting point for the future realization of scalable quantum computation, but may also find application in magnetic memory or low-power electronic devices. This thesis reports on the pulsed laser deposition of high-quality heteroepitaxial (001)-oriented Na2IrO3 thin films with well-defined in-plane epitaxial relationship on 5-by-5 and 10-by-10 square millimeter single-crystalline sapphire, YAlO3 and zinc oxide substrates. Three-dimensional Mott variable range hopping is the dominant conduction mechanism between 40 and 300 K. Moreover, a signature of the proposed topological insulator phase is found in magnetoresistance by observation of the weak antilocalization effect that is associated with topological surafce states. Compared to single crystals, a smaller, 200-meV optical gap in Na2IrO3 thin films is found by Fourier-transform infrared transmission spectroscopy.

The layered honeycomb lattice iridate Na2IrO3 is a novel candidate material for either a topological insulator or spin liquid. These states of matter are one possible starting point for the future realization of scalable quantum computation, but may also find application in magnetic memory or low-power electronic devices. This thesis reports on the pulsed laser deposition of high-quality heteroepitaxial (001)-oriented Na2IrO3 thin films with well-defined in-plane epitaxial relationship on 5-by-5 and 10-by-10 square millimeter single-crystalline sapphire, YAlO3 and zinc oxide substrates. Three-dimensional Mott variable range hopping is the dominant conduction mechanism between 40 and 300 K. Moreover, a signature of the proposed topological insulator phase is found in magnetoresistance by observation of the weak antilocalization effect that is associated with topological surafce states. Compared to single crystals, a smaller, 200-meV optical gap in Na2IrO3 thin films is found by Fourier-transform infrared transmission spectroscopy.