Crystal Phase Distribution and Ferroelectricity in Ultrathin HfO 2 –ZrO 2 Bilayers
Abstract
(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 developmentmore »
- Authors:
-
[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
- Publication Date:
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1561364
- Grant/Contract Number:
- AC02-76SF00515
- Resource Type:
- Publisher's Accepted Manuscript
- Journal Name:
- Physica Status Solidi B. Basic Solid State Physics
- Additional Journal Information:
- Journal Name: Physica Status Solidi B. Basic Solid State Physics Journal Volume: 257 Journal Issue: 1; Journal ID: ISSN 0370-1972
- Publisher:
- Wiley Blackwell (John Wiley & Sons)
- Country of Publication:
- Germany
- Language:
- English
Citation Formats
McBriarty, Martin E., Narasimhan, Vijay K., Weeks, Stephen L., Pal, Ashish, Fang, Huazhi, Petach, Trevor A., Mehta, Apurva, Davis, Ryan C., Barabash, Sergey V., and Littau, Karl A. Crystal Phase Distribution and Ferroelectricity in Ultrathin HfO 2 –ZrO 2 Bilayers. Germany: N. p., 2019.
Web. doi:10.1002/pssb.201900285.
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. Crystal Phase Distribution and Ferroelectricity in Ultrathin HfO 2 –ZrO 2 Bilayers. Germany. https://doi.org/10.1002/pssb.201900285
McBriarty, Martin E., Narasimhan, Vijay K., Weeks, Stephen L., Pal, Ashish, Fang, Huazhi, Petach, Trevor A., Mehta, Apurva, Davis, Ryan C., Barabash, Sergey V., and Littau, Karl A. Wed .
"Crystal Phase Distribution and Ferroelectricity in Ultrathin HfO 2 –ZrO 2 Bilayers". Germany. https://doi.org/10.1002/pssb.201900285.
@article{osti_1561364,
title = {Crystal Phase Distribution and Ferroelectricity in Ultrathin HfO 2 –ZrO 2 Bilayers},
author = {McBriarty, Martin E. and Narasimhan, Vijay K. and Weeks, Stephen L. and Pal, Ashish and Fang, Huazhi and Petach, Trevor A. and Mehta, Apurva and Davis, Ryan C. and Barabash, Sergey V. and Littau, Karl A.},
abstractNote = {(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.},
doi = {10.1002/pssb.201900285},
journal = {Physica Status Solidi B. Basic Solid State Physics},
number = 1,
volume = 257,
place = {Germany},
year = {Wed Sep 11 00:00:00 EDT 2019},
month = {Wed Sep 11 00:00:00 EDT 2019}
}
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