Crystal Phase Distribution and Ferroelectricity in Ultrathin HfO 2 –ZrO 2 Bilayers

McBriarty, Martin E.; Narasimhan, Vijay K.; Weeks, Stephen L.; Pal, Ashish; Fang, Huazhi; Petach, Trevor A.; Mehta, Apurva; Davis, Ryan C.; Barabash, Sergey V.; Littau, Karl A.

doi:10.1002/pssb.201900285

Title: Crystal Phase Distribution and Ferroelectricity in Ultrathin HfO ₂ –ZrO ₂ Bilayers

Journal Article · Wed Sep 11 00:00:00 EDT 2019 · Physica Status Solidi B. Basic Solid State Physics

DOI:https://doi.org/10.1002/pssb.201900285· OSTI ID:1561364

^[1]; Narasimhan, Vijay K. ^[1]; Weeks, Stephen L. ^[1]; Pal, Ashish ^[1]; Fang, Huazhi ^[1]; Petach, Trevor A. ^[2]; Mehta, Apurva ^[2]; Davis, Ryan C. ^[2]; Barabash, Sergey V. ^[1]; Littau, Karl A. ^[1]

Technology Group Intermolecular, Inc. 3011 N. 1st Street San Jose CA 95134 USA
Stanford Synchrotron Radiation Lightsource SLAC National Accelerator Center Menlo Park CA 94025 USA

(Hf,Zr)O ₂ ultrathin films are used as ferroelectric layers in emerging digital logic and nonvolatile memory devices. The ferroelectric properties of (Hf,Zr)O ₂ can be improved by interface engineering, such as the formation of nanolaminates with distinct HfO ₂ and ZrO ₂ layers. Herein, the ferroelectric performance of HfO ₂ –ZrO ₂ ultrathin bilayer devices is shown to depend on the stacking order of HfO ₂ and ZrO ₂ , which affects the quantity of the noncentrosymmetric orthorhombic Pca 2 ₁ crystal phase. By combining X‐ray diffraction with a novel extended X‐ray absorption fine structure (EXAFS) analysis procedure, the orthorhombic, tetragonal, and monoclinic phase fractions are quantified for bilayers composed of 3 nm HfO ₂ and 3 nm ZrO ₂ . A significantly larger orthorhombic ZrO ₂ phase fraction is found when ZrO ₂ has an unconstrained surface during annealing, whereas the presence of a ZrO ₂ interface with the substrate results in a substantial tetragonal ZrO ₂ phase fraction and a 2.4× smaller remanent polarization. HfO ₂ is found to be less susceptible than ZrO ₂ to crystal phase templating. The methods presented herein enable mechanistic studies of ferroelectric wake‐up, fatigue, and processing effects in (Hf,Zr)O ₂ films, accelerating the development of electronic devices that rely on ferroelectric oxides.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 1561364

Journal Information:: Physica Status Solidi B. Basic Solid State Physics, Journal Name: Physica Status Solidi B. Basic Solid State Physics Vol. 257 Journal Issue: 1; ISSN 0370-1972

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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Cited by: 17 works

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