Plasma-Assisted Atomic Layer Deposition of SrTiO₃: Stoichiometry and Crystallinity Studied by Spectroscopic Ellipsometry

Strontium titanate (SrTiO 3 , STO) films were deposited by plasma-assisted ALD using cyclopentadienyl-based Sr-and Ti-precursors with O 2 plasma as the oxidizing agent. Spectroscopic ellipsometry (SE) was employed to determine the thickness and the optical properties of the layers. As determined from Rutherford backscattering spectrometry (RBS), [Sr]/([Sr]+[Ti]) ratios ranging from 0.42 to 0.68 were achieved for 30-40 nm thick films by tuning the [SrO]/[TiO 2 ] ALD cycle ratio. Films deposited at 250 C were amorphous and required post-deposition annealing to crystallize into the ultrahigh-k perovskite structure. The crystallinity of the films after rapid thermal annealing strongly depended on the film composition as observed by X-ray diffraction measurements. Using RBS data for a set of as-deposited samples, an optical constant library was built to determine the film stoichiometry from SE directly for the amorphous as-deposited films. After rapid thermal annealing the crystalline phase could be determined from the position of critical points of the measured dielectric function and the estimation of the stoichiometry was also possible for crystallized layers. These results open up a new way to use SE as a real-time characterization method to monitor and tune the STO film composition and crystallinity.