Correlation between ferroelectricity and ferroelectric orthorhombic phase of HfxZr1-xO2 thin films using synchrotron x-ray analysis

Onaya, Takashi; Nabatame, Toshihide; Jung, Yong Chan; Hernandez-Arriaga, Heber; Mohan, Jaidah; Kim, Harrison Sejoon; Sawamoto, Naomi; Nam, Chang-Yong; Tsai, Esther R.; Nagata, Takahiro; Kim, Jiyoung; Ogura, Atsushi

doi:10.1063/5.0035848

Correlation between ferroelectricity and ferroelectric orthorhombic phase of Hf_xZr_1-xO₂ thin films using synchrotron x-ray analysis

Journal Article · Fri Mar 26 00:00:00 EDT 2021 · APL Materials

DOI:https://doi.org/10.1063/5.0035848· OSTI ID:1776535

^[1]; Nabatame, Toshihide ^[2]; ^[3]; Hernandez-Arriaga, Heber ^[3]; ^[3]; ^[3]; Sawamoto, Naomi ^[4]; ^[5]; ^[5]; ^[2]; ^[3]; ^[6]

Meiji Univ., Kawasaki (Japan); National Inst. for Materials Science (NIMS), Tsukuba (Japan); Univ. of Texas at Dallas, Richardson, TX (United States)
National Inst. for Materials Science (NIMS), Tsukuba (Japan)
Univ. of Texas at Dallas, Richardson, TX (United States)
Meiji Univ., Kawasaki (Japan). Meiji Renewable Energy Lab.
Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
Meiji Univ., Kawasaki (Japan); Meiji Univ., Kawasaki (Japan). Meiji Renewable Energy Lab.

The change in the interplanar spacing (d-spacing) including the ferroelectric orthorhombic (O) phase in the low-temperature fabricated Hf_xZr_1-xO₂ (HZO) films was studied using synchrotron grazing-incidence wide-angle x-ray scattering analysis. The 10-nm-thick HZO films were fabricated by thermal and plasma-enhanced atomic layer deposition (TH- and PE-ALD) methods using H₂O gas and O₂ plasma as oxidants, respectively, and a post-metallization annealing (PMA) was performed at 300–400 °C. The d-spacing of the mixture of (111)-, (101)-, and (111)-planes of O, tetragonal (T), and cubic (C) phases, respectively, for the TH- and PE-ALD HZO films increased up to 2.99 Å with an increase in PMA temperature, while the d-spacing estimated by conventional x-ray diffraction was 2.92 Å regardless of the PMA temperature. The remanent polarization (2P_r = P_r⁺ - P_r^-) of the HZO films increased as the PMA temperature increased. It is clear that the 2P_r value satisfied a linear relationship as a function of the d-spacing of O(111)/T(101)/C(111) phases. Furthermore, the wake-up effect was found to depend on the ferroelectric O phase formation. The wake-up effect was significantly reduced in both the TH- and PE-ALD HZO films after the PMA at 400 °C due to the increase in the ferroelectric O phase formation. The leakage current density (J)–electric field properties of the PE-ALD HZO film with the lowest d-spacing were divided into three steps, such as low, middle, and large J values, in the wake-up (10³ cycles), pristine (10⁰ cycle), and fatigue (10⁷ cycles) states, respectively. Therefore, an analysis of the ferroelectric O phase is very important for understanding the ferroelectricity including endurance.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: JSPS KAKENHI; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012704

OSTI ID:: 1776535

Report Number(s):: BNL--221229-2021-JAAM

Journal Information:: APL Materials, Journal Name: APL Materials Journal Issue: 3 Vol. 9; ISSN 2166-532X

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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Correlation between ferroelectricity and ferroelectric orthorhombic phase of HfxZr1-xO2 thin films using synchrotron x-ray analysis

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References (48)

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Correlation between ferroelectricity and ferroelectric orthorhombic phase of Hf_xZr_1-xO₂ thin films using synchrotron x-ray analysis