Kinetically stabilized ferroelectricity in bulk single-crystalline HfO2:Y

Xu, Xianghan; Huang, Fei-Ting; Qi, Yubo; Rabe, Karin M.; Obeysekera, Dimuthu; Chu, Ming-Wen; Cheong, Sang-Wook; Singh, Sobhit; Yang, Junjie

doi:10.1038/s41563-020-00897-x

Title: Kinetically stabilized ferroelectricity in bulk single-crystalline HfO₂:Y

Journal Article · Mon Jan 25 00:00:00 EST 2021 · Nature Materials

DOI:https://doi.org/10.1038/s41563-020-00897-x· OSTI ID:1798576

^[1]; Huang, Fei-Ting ^[1]; Qi, Yubo ^[1]; Rabe, Karin M. ^[1];

^[2]; Chu, Ming-Wen ^[3]; Cheong, Sang-Wook ^[1];

^[4];

^[2]

Rutgers Univ., Piscataway, NJ (United States)
New Jersey Institute of Technology, Newark, NJ (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
National Taiwan Univ., Taipei (Taiwan)
Rutgers Univ., Piscataway, NJ (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

HfO₂, a simple binary oxide, exhibits ultra-scalable ferroelectricity integrable into silicon technology. This material has a polymorphic nature, with the polar orthorhombic (Pbc2₁) form in ultrathin films regarded as the plausible cause of ferroelectricity but thought not to be attainable in bulk crystals. In this work, using a state-of-the-art laser-diode-heated floating zone technique, we report the Pbc2₁ phase and ferroelectricity in bulk single-crystalline HfO₂:Y as well as the presence of the antipolar Pbca phase at different Y concentrations. Neutron diffraction and atomic imaging demonstrate (anti)polar crystallographic signatures and abundant 90°/180° ferroelectric domains in addition to switchable polarization with negligible wake-up effects. Density-functional-theory calculations indicate that the yttrium doping and rapid cooling are the key factors for stabilization of the desired phase in bulk. Our observations provide insights into the polymorphic nature and phase control of HfO₂, remove the upper size limit for ferroelectricity and suggest directions towards next-generation ferroelectric devices.

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Research Organization:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); Gordon and Betty Moore Foundation; US Department of the Navy, Office of Naval Research (ONR)

Grant/Contract Number:: AC05-00OR22725; GBMF6402; N00014-17-1-2770

OSTI ID:: 1798576

Journal Information:: Nature Materials, Vol. 20, Issue 6; ISSN 1476-1122

Publisher:: Springer Nature - Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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