Abstract

For the first time, the dynamic process of orthorhombic (o-) phase emergence during rapid thermal annealing in polycrystalline Hf <inf xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">0.5</inf> Zr <inf xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">0.5</inf> O <inf xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</inf> (HZO) ferroelectric film was directly visualized though in-situ spherical aberration corrected transmission electron microscopy technique. We have the following main observations: (1) o-phase nucleates from centrosymmetric tetragonal (t-) phase at top TiN/HZO interface where the oxygen vacancy (Vo) concentration is rich, identifying that Vo is helpful to lower the free energy of o-phase; (2) o-phase appears in both heating up and cooling down stages. The o-phase formed in the heating stage rapidly transforms into t-phase again as the temperature further increasing, and the one formed in the cooling stage is retained. These findings provide solid evidence on the o-phase origin in fluorite-type ferroelectric materials.

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