Ferroelectric orthorhombic ZrO2 thin films achieved through nanosecond laser annealing

A new approach for the stabilization of the ferroelectric orthorhombic ZrO2 films is demonstrated through nanosecond laser annealing (NLA) of as-deposited Si/SiOx/W(14 nm)/ZrO2(8 nm)/W(22 nm), grown by ion beam sputtering at low temperatures. The NLA process optimization is guided by COMSOL multiphysics simulations. The films annealed under the optimized conditions reveal the presence of the orthorhombic phase, as confirmed by X-ray diffraction, electron backscatter diffraction, and transmission electron microscopy. Macroscopic polarization-electric field hysteresis loops show ferroelectric behavior, with saturation polarization of 12.8 mu C cm(-2), remnant polarization of 12.7 mu C cm(-2) and coercive field of 1.2 MV cm(-1). The films exhibit a wake-up effect that is attributed to the migration of point defects, such as oxygen vacancies, and/or a transition from nonferroelectric (monoclinic and tetragonal phase) to the ferroelectric orthorhombic phase. The capacitors demonstrate a stable polarization with an endurance of 6.0 x 10(5) cycles, demonstrating the potential of the NLA process for the fabrication of ferroelectric memory devices with high polarization, low coercive field, and high cycling stability.A.P.S.C. and M.C.I. contributed equally to this work. This work was supported by the Portuguese Foundation for Science and Technology (FCT) in the framework of the Strategic Funding Contract UIDB/04650/2020. This work has received funding from the European Union's Horizon 2020 research and innovation program under grant agreement No 958174 (M-ERA-NET3/0003/2021-NanOx4EStor). M. C. I. and C. G. acknowledge the financial support by a grant of the Ministry of Research, Innovation and Digitization, CNCS/CCCDI - UEFISCDI, project number COFUND-M-ERANET-3-NanOx4Estor, within PNCDI III and POC 332/390008/29.12.2020-SMIS 109522. The authors acknowledge the CERIC-ERIC Consortium for access to experimental facilities and financial support under proposals 20202037, 20202038, and 20192055. The authors would also like to thank Jose Santos for technical support in the Thin Film Laboratory at CF-UM-UP. J.L.M-D. thanks the ERC grant, EU-H2020-ERC-ADG #882929, EROS. And the Royal Academy of Engineering, grant CIET1819_24. MOH thanks the Herchel Smith foundation of Cambridge for a research fellowship. This work made use of the University of Cambridge Wolfson Electron Microscopy Suite