Atomic layer deposition (ALD) of ZrO2-Gd2O3 nanolaminates and mixtures was investigated for the preparation of a high permittivity dielectric material. Variation in the relative number of ALD cycles for constituent oxides allowed one to obtain films with controlled composition. Pure ZrO2 films possessed monoclinic and higher permittivity cubic or tetragonal phases, whereas the inclusion of Gd2O3 resulted in the disappearance of the monoclinic phase. Changes in phase composition were accompanied with increased permittivity of mixtures and laminates with low Gd content. Further increase in the lower permittivity Gd2O3 content above 3.4 cat. % resulted in the decreased permittivity of the mixtures. Leakage currents generally decreased with increasing Gd content, whereby laminated structures demonstrated smaller leakage currents than mixed films at a comparable Gd content. Concerning the bottom electrode materials, the best results in terms of permittivity and leakage currents were achieved with Ru, allowing a capacitance equivalent oxide thickness of similar to 1 nm and a current density of 3 X 10(-8) A/cm(2) at 1 V. Charge storage values up to 60 nC/mm(2) were obtained for mixtures and laminates with thickness below 30 nm. In general, at electric fields below 2-3 MV/cm, normal and trap-compensated Poole-Frenkel conduction mechanisms were competing, whereas at higher fields, Fowler-Nordheim and/or trap-assisted tunneling started to dominate. (C) 2010 The Electrochemical Society. [DOI: 10.1149/1.3478117] All rights reserved.