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 $\mathrm{FE}$-${\mathrm{Hf}\mathrm{O}}_{2}$.
Authors
- Fachen Liu
- Jinfeng Kang (ORCID: https://orcid.org/0000-0002-6286-0423)
- Xiangxiang Ding (ORCID: https://orcid.org/0000-0001-7719-7508)
- Yudi Zhao (ORCID: https://orcid.org/0000-0002-8444-763X)
- Chenxi Yu (ORCID: https://orcid.org/0000-0002-2813-9528)
- Peng Huang (ORCID: https://orcid.org/0000-0003-3280-0099)
- Peng Gao (ORCID: https://orcid.org/0000-0002-1290-6972)
- Fei Liu (ORCID: https://orcid.org/0000-0003-3212-7594)
- Haolin Li (ORCID: https://orcid.org/0000-0002-0478-3538)
- Lifeng Liu (ORCID: https://orcid.org/0000-0002-0187-9243)
- Jun Xu (ORCID: https://orcid.org/0000-0003-3507-0159)
- Xujin Song (ORCID: https://orcid.org/0009-0006-1037-1851)
- Jingmin Zhang (ORCID: https://orcid.org/0000-0002-2765-6574)
- Mingqiang Li (ORCID: https://orcid.org/0000-0001-9854-2251)
- Wanwang Yang (ORCID: https://orcid.org/0000-0002-9387-1731)
- Haili Ma
- Xiaorui Hao
Institutions
- Peking University (CN)
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
- National Natural Science Foundation of China
- National Key Research and Development Program of China