Thin stacks comprised of alternating layers of Ta 2 O 5 /HfO 2 , Ta 2 O 5 /ZrO 2 , and ZrO 2 /HfO 2 were investigated as high-permittivity insulators for possible gate dielectric applications. These thin layers were deposited on silicon substrates using atomic layer deposition. Nanolaminates with silicon oxide equivalent thickness of about 2 nm had dielectric constants of around ten and leakage current densities at 1 MV/cm of around 10 Ϫ8 A/cm 2 . Of the three kinds of nanolaminates investigated, ZrO 2 /HfO 2 structures showed the highest breakdown field and the lowest leakage current.The continuous downscaling of metal-oxide-semiconductor field effect transistors ͑MOSFETs͒ requires a corresponding reduction of the gate dielectric thickness. As a result of this reduction, direct tunneling current through the silicon dioxide gate dielectric is becoming a very serious issue. The current generation of MOSFETs with channel length of 0.18 m requires a proportional decrease in the oxide equivalent thickness of the gate insulator to less than 3 nm. A major limiting factor in transistor scaling beyond the current 0.18 m design rules has been the difficulty of growing highquality, ultrathin oxides as the tunneling limit of 2.5 nm for SiO 2 is approached and gate leakage currents exceed 1 A/cm 2 . Furthermore, SiO 2 is not a good diffusion barrier for gate electrode dopants, such as boron. Even with nitrogen incorporation, 1,2 it is difficult to utilize ultrathin nitrided oxides for sub-quarter-micrometer technologies due to high tunneling current and rough Si-SiO 2 interface. Therefore, when the SiO 2 thickness is reduced to below 2 nm, alternate high-permittivity ͑k͒ dielectrics such as Ta 2 O 5 , HfO 2 , and ZrO 2 must be considered. Ta 2 O 5 has been investigated as the capacitor dielectric in gigabit dynamic random access memory chips ͑DRAMs͒. 3-5 Recently MOSFET devices have also been fabricated using high-k thin films including Ta 2 O 5 , HfO 2 , and ZrO 2 . 6-9 One major obstacle in using high-k materials is that a solid material with higher permittivity tends to have a narrower bandgap. This is deduced from a reduced cohesive force according to the quantummechanical consideration, 10 thereby suffering from a larger leakage current. We have previously reported a remarkable improvement of binary high-permittivity oxides by preparing nanolaminates which were composed of alternate layers of Ta 2 O 5 /HfO 2 , Ta 2 O 5 /ZrO 2 , and ZrO 2 /HfO 2 . 11 In this paper we present our recent results on properties of much thinner nanolaminates as dielectrics in metaloxide-semiconductor capacitor ͑MOSCAP͒ structures.These films were deposited using the unique self-limiting growth process of atomic layer deposition ͑ALD͒ that allows film growth one atomic layer at a time from multiple source materials at relatively low temperatures. In this process one reactant at a time is injected into the growth area, and following surface reaction, excess species and by-products are purged with an inert gas. As a result, films are grown by se...