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We report that an energetic plasma process is extremely effective inenlarging the unit cell volume and ferroelectric distortion of theferroelectric oxides, resulting in a significant increase in its Tc. Wedemonstrate experimentally that c-axis oriented BaTiO3 films can be depositeddirectly on quartz glass and Si substrates using such a process and that thematerial shows an approximately 5% expansion of its unit cell volume andapproximately 4 times the ferroelectric tetragonal distortion of the bulkcrystals. Such a frozen negative pressure results in a Tc value that isapproximately 580 K higher than that of bulk single crystals, providing a widerange of operating temperatures for the devices. The present results suggest anapproach to producing ferroelectric oxides with unique properties that might beextended to ferromagnetic or superconductor oxides and demonstrate a route to alead-free ferroelectric oxide for capacitive, ferroelectric memory, andelectro-optical devices.

High-Tc BaTiO3 ferroelectric films with frozen negative pressure states