Insights into the origin of robust ferroelectricity in <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline" overflow="scroll"><mml:msub><mml:mrow><mml:mi>Hf</mml:mi><mml:mi mathvariant="normal">O</mml:mi></mml:mrow><mml:mn>2</mml

${\mathrm{Hf}\mathrm{O}}_{2}$-based ferroelectrics ($\mathrm{FE}\text{\ensuremath{-}}{\mathrm{Hf}\mathrm{O}}_{2}$) have triggered extensive research interest because they are promising materials for beyond-Moore electronic device applications. However, the origin of ferroelectricity in ${\mathrm{Hf}\mathrm{O}}_{2}$-based ferroelectrics remains elusive. Here, we demonstrate that the ordered oxygen vacancies (${\mathrm{V}}_{\mathrm{O}}$) in $\mathrm{FE}$-${\mathrm{Hf}\mathrm{O}}_{2}$ thin films contribute to ferroelectricity through the formation of a stable-polar phase. In $\mathrm{FE}$-${\mathrm{Hf}\mathrm{O}}_{2}$ thin films, oxygen vacancy (${\mathrm{V}}_{\mathrm{O}}$) defects induce local electric dipoles and the ordered ${\mathrm{V}}_{\mathrm{O}}$ distribution results in the stable-polar phases. Using first-principles calculations, a thermodynamically stable-polar phase ${M}_{1}$ with the spontaneous polarization of 27 \textmu{}C/${\mathrm{cm}}^{2}$ is predicted in monocliniclike ${\mathrm{Hf}}_{4}{\mathrm{Zr}}_{4}{\mathrm{O}}_{15}$ structures. Moreover, the predicted ${M}_{1}$ structures are directly visualized in ${\mathrm{Hf}}_{0.5}{\mathrm{Zr}}_{0.5}{\mathrm{O}}_{2\ensuremath{-}\ensuremath{\delta}}$ (HZO) ferroelectric thin films using spherical aberration (Cs)-corrected scanning transmission electron microscopy. The proposed mechanism for ${\mathrm{V}}_{\mathrm{O}}$-induced order-disorder ferroelectricity in $\mathrm{FE}$-${\mathrm{Hf}\mathrm{O}}_{2}$ opens a new pathway to explore the underlying physics of the ferroelectric characteristics in $\mathrm{FE}$-${\mathrm{Hf}\mathrm{O}}_{2}$.

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Publication Details

Journal
Physical Review Applied
Published
2024-08-09
DOI
https://doi.org/10.1103/physrevapplied.22.024028
Citations
7
Primary Topic
Ferroelectric and Negative Capacitance Devices
Type
article
Field-Weighted Citation Impact
1.46

Funders

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article

Insights into the origin of robust ferroelectricity in <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline" overflow="scroll"><mml:msub><mml:mrow><mml:mi>Hf</mml:mi><mml:mi mathvariant="normal">O</mml:mi></mml:mrow><mml:mn>2</mml

Fachen Liu, Jinfeng Kang, Xiangxiang Ding, Yudi Zhao et al.
7 citations
Physical Review Applied
Ferroelectric and Negative Capacitance Devices
1.46
article

Insights into the origin of robust ferroelectricity in <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline" overflow="scroll"><mml:msub><mml:mrow><mml:mi>Hf</mml:mi><mml:mi mathvariant="normal">O</mml:mi></mml:mrow><mml:mn>2</mml

Fachen Liu, Jinfeng Kang, Xiangxiang Ding, Yudi Zhao, Chenxi Yu, Peng Huang, Peng Gao, Fei Liu, Haolin Li, Lifeng Liu, Jun Xu, Xujin Song, Jingmin Zhang, Mingqiang Li, Wanwang Yang, Haili Ma, Xiaorui Hao
article en
7 citations

Abstract

${\mathrm{Hf}\mathrm{O}}_{2}$-based ferroelectrics ($\mathrm{FE}\text{\ensuremath{-}}{\mathrm{Hf}\mathrm{O}}_{2}$) have triggered extensive research interest because they are promising materials for beyond-Moore electronic device applications. However, the origin of ferroelectricity in ${\mathrm{Hf}\mathrm{O}}_{2}$-based ferroelectrics remains elusive. Here, we demonstrate that the ordered oxygen vacancies (${\mathrm{V}}_{\mathrm{O}}$) in $\mathrm{FE}$-${\mathrm{Hf}\mathrm{O}}_{2}$ thin films contribute to ferroelectricity through the formation of a stable-polar phase. In $\mathrm{FE}$-${\mathrm{Hf}\mathrm{O}}_{2}$ thin films, oxygen vacancy (${\mathrm{V}}_{\mathrm{O}}$) defects induce local electric dipoles and the ordered ${\mathrm{V}}_{\mathrm{O}}$ distribution results in the stable-polar phases. Using first-principles calculations, a thermodynamically stable-polar phase ${M}_{1}$ with the spontaneous polarization of 27 \textmu{}C/${\mathrm{cm}}^{2}$ is predicted in monocliniclike ${\mathrm{Hf}}_{4}{\mathrm{Zr}}_{4}{\mathrm{O}}_{15}$ structures. Moreover, the predicted ${M}_{1}$ structures are directly visualized in ${\mathrm{Hf}}_{0.5}{\mathrm{Zr}}_{0.5}{\mathrm{O}}_{2\ensuremath{-}\ensuremath{\delta}}$ (HZO) ferroelectric thin films using spherical aberration (Cs)-corrected scanning transmission electron microscopy. The proposed mechanism for ${\mathrm{V}}_{\mathrm{O}}$-induced order-disorder ferroelectricity in $\mathrm{FE}$-${\mathrm{Hf}\mathrm{O}}_{2}$ opens a new pathway to explore the underlying physics of the ferroelectric characteristics in $\mathrm{FE}$-${\mathrm{Hf}\mathrm{O}}_{2}$.

Physical Review AppliedVol. 22(2)
Peking University (CN)
National Natural Science Foundation of China, National Key Research and Development Program of China
Openalex Percentile: Top 18%
Ferroelectric and Negative Capacitance Devices
1.46
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