Atomic Layer Growth of Rutile TiO2 Films with Ultrahigh Dielectric Constants via Crystal Orientation Engineering

In general, the electronic and optical properties of oxide films can significantly benefit from highly textured crystallinity. However, oxide films grown by atomic layer deposition (ALD), a powerful technique for the synthesis of high-quality, nanoscale thin films, usually exhibit amorphous or randomly oriented polycrystalline phases. Here, we demonstrate the growth of highly textured rutile phase ALD TiO₂ films through rational substrate design. Both a- and c-axis preferentially oriented TiO₂ films are obtained by varying the lattice parameters of the initial ALD growth surface. Under optimized conditions, we find that it is possible to deposit high-quality, c-axis preferentially aligned TiO₂ films with a bulk dielectric constant approaching 185, rivaling the single crystal limit. These films display a remarkably high dielectric constant of 117 despite thin thickness of 5.2 nm. Moreover, the addition of a single doping sequence of Al₂O₃ successfully suppresses leakage currents to levels compatible with modern dynamic random access memory cells, all the while maintaining the high bulk dielectric constant of 137. These results clearly highlight the prospect of utilizing crystal orientation engineering in ALD thin films for emerging semiconductor devices.