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In this paper, an approach using native SiO2 to make amorphous higher dielectric constant films based on the Y2O3-TiO2/SiO2/Si compositional spread libraries by combinatorial pulsed laser deposition is reported. The key feature of the experiment is that combinatorial methodology is used to quickly screen the potential high-dielectric-constant films out of a large composition parameter space. Scanning X-ray microdiffractometry and high-resolution transmission electron microscopy results show that the TiO2-rich end is amorphous after 500°C anneal. A wide composition range near the TiO2-rich end, exhibiting amorphousness, dielectric constants of 30-50, and reasonably low JL (<; 10-5 A/cm2), may be of great interest for a gate-last process flow for advanced gate stacks.