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Title: On the Origin of the Large Remanent Polarization in La:HfO2

Abstract

We report that the outstanding remanent polarization of 40 µC cm–2 reported for a 10 nm thin La:HfO2 film in 2013 has attracted much attention. However, up to now, no explanation for this large remanent polarization has been presented. Density functional theory and X-ray diffraction are used to shine light onto three major aspects that impact the macroscopically observed remanent polarization: phase fraction, spontaneous polarization, and crystallographic texture. Density functional theory calculations show that the spontaneous polarization (Ps) of La:HfO2 is indeed a bit larger than for other HfO2-or ZrO2-based compounds; however, the Ps is not large enough to explain the observed differences in remanent polarization. While neither phase fractions nor spontaneous polarization nor strain are significantly different from those in other HfO2 films, a prominent 020/002 texture distinguishes La doped from other HfO2-based ferroelectric films. Angular-dependent diffraction data provide a pathway to calculate the theoretically expected remanent polarization, which is in agreement with the experimental observations. Finally, an interplay of the in-plane strain and texture is proposed to impact the formation of the ferroelectric phase during annealing. Lastly, further aspects of the special role of La as a dopant are collected and discussed to motivate future research.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3];  [4]; ORCiD logo [5];  [5];  [6]; ORCiD logo [7]; ORCiD logo [4]
  1. NaMLab gGmbH, Dresden (Germany); Luxembourg Institute of Science and Technology (LIST), Belvaux (Luxembourg)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. NaMLab gGmbH, Dresden (Germany); Pusan National Univ., Geumjeong‐gu, Busan (Republic of Korea)
  4. NaMLab gGmbH, Dresden (Germany)
  5. Munich Univ. of Applied Sciences (Germany)
  6. North Carolina State Univ., Raleigh, NC (United States)
  7. NaMLab gGmbH, Dresden (Germany); Inst. of Semiconductors and Microsystems TU Dresden (Germany)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1607176
Alternate Identifier(s):
OSTI ID: 1562972
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Electronic Materials
Additional Journal Information:
Journal Volume: 5; Journal Issue: 12; Journal ID: ISSN 2199-160X
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; ferroelectrics; HfO2; stress; texture; XRD

Citation Formats

Schenk, Tony, Fancher, Chris M., Park, Min Hyuk, Richter, Claudia, Künneth, Christopher, Kersch, Alfred, Jones, Jacob L., Mikolajick, Thomas, and Schroeder, Uwe. On the Origin of the Large Remanent Polarization in La:HfO2. United States: N. p., 2019. Web. https://doi.org/10.1002/aelm.201900303.
Schenk, Tony, Fancher, Chris M., Park, Min Hyuk, Richter, Claudia, Künneth, Christopher, Kersch, Alfred, Jones, Jacob L., Mikolajick, Thomas, & Schroeder, Uwe. On the Origin of the Large Remanent Polarization in La:HfO2. United States. https://doi.org/10.1002/aelm.201900303
Schenk, Tony, Fancher, Chris M., Park, Min Hyuk, Richter, Claudia, Künneth, Christopher, Kersch, Alfred, Jones, Jacob L., Mikolajick, Thomas, and Schroeder, Uwe. Thu . "On the Origin of the Large Remanent Polarization in La:HfO2". United States. https://doi.org/10.1002/aelm.201900303. https://www.osti.gov/servlets/purl/1607176.
@article{osti_1607176,
title = {On the Origin of the Large Remanent Polarization in La:HfO2},
author = {Schenk, Tony and Fancher, Chris M. and Park, Min Hyuk and Richter, Claudia and Künneth, Christopher and Kersch, Alfred and Jones, Jacob L. and Mikolajick, Thomas and Schroeder, Uwe},
abstractNote = {We report that the outstanding remanent polarization of 40 µC cm–2 reported for a 10 nm thin La:HfO2 film in 2013 has attracted much attention. However, up to now, no explanation for this large remanent polarization has been presented. Density functional theory and X-ray diffraction are used to shine light onto three major aspects that impact the macroscopically observed remanent polarization: phase fraction, spontaneous polarization, and crystallographic texture. Density functional theory calculations show that the spontaneous polarization (Ps) of La:HfO2 is indeed a bit larger than for other HfO2-or ZrO2-based compounds; however, the Ps is not large enough to explain the observed differences in remanent polarization. While neither phase fractions nor spontaneous polarization nor strain are significantly different from those in other HfO2 films, a prominent 020/002 texture distinguishes La doped from other HfO2-based ferroelectric films. Angular-dependent diffraction data provide a pathway to calculate the theoretically expected remanent polarization, which is in agreement with the experimental observations. Finally, an interplay of the in-plane strain and texture is proposed to impact the formation of the ferroelectric phase during annealing. Lastly, further aspects of the special role of La as a dopant are collected and discussed to motivate future research.},
doi = {10.1002/aelm.201900303},
journal = {Advanced Electronic Materials},
number = 12,
volume = 5,
place = {United States},
year = {2019},
month = {9}
}

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