Ultrahigh Dielectric Permittivity of a Micron-Sized HfZrO Thin-Film Capacitor After Missing of a Mixed Tetragonal Phase.

Innovative use of HfO-based high-dielectric-permittivity materials could enable their integration into few-nanometre-scale devices for storing substantial quantities of electrical charges, which have received widespread applications in high-storage-density dynamic random access memory and energy-efficient complementary metal-oxide-semiconductor devices. During bipolar high electric-field cycling in numbers close to dielectric breakdown, the dielectric permittivity suddenly increases by 30 times after oxygen-vacancy ordering and ferroelectric-to-nonferroelectric phase transition of near-edge plasma-treated HfZrO thin-film capacitors. Here we report a much higher dielectric permittivity of 1466 during downscaling of the capacitor into the diameter of 3.85 μm when the ferroelectricity suddenly disappears without high-field cycling. The stored charge density is as high as 183 μC cm at an operating voltage/time of 1.2 V/50 ns at cycle numbers of more than 10 without inducing dielectric breakdown. The study of synchrotron X-ray micro-diffraction patterns show missing of a mixed tetragonal phase. The image of electron energy loss spectroscopy shows the preferred oxygen-vacancy accumulation at the regions near top/bottom electrodes as well as grain boundaries. The ultrahigh dielectric-permittivity material enables high-density integration of extremely scaled logic and memory devices in the future.