Polarization switching in ferroelectric HfO2 from first-principles lattice mode analysis

Yubo Qi; Sobhit Singh; Karin M. Rabe

doi:10.1103/PhysRevB.111.134106

Polarization switching in ferroelectric HfO₂ from first-principles lattice mode analysis

Yubo Qi, Sobhit Singh, Karin M. Rabe

School of Arts and Sciences, New High Energy Theory Center

Rutgers, The State University

Research output: Contribution to journal › Article › peer-review

Abstract

In this paper, we introduce a first-principles-based lattice mode analysis method to investigate the competition between different polarization switching paths in HfO₂. Because the stability of the polar orthorhombic Pca21 phase of HfO₂ arises from a trilinear coupling, polarization switching requires the flipping of not only the polar Γ15Z mode, but also at least one zone-boundary antipolar mode. This means that each polarization state has multiple variants, leading to multiple possible switching paths connecting up- and down-polarized states, which can be systemically enumerated within this framework for efficient identification of the optimal switching path. Our lattice mode analysis also explains why the activation energy of propagation of the most widely studied domain-wall structure in HfO₂, which requires the reversal of the X2- mode, is much larger than that of propagation of domain-wall structures with a uniform sign for the X2- mode. This approach deepens our understanding of distinctive properties of ferroelectric HfO₂ related to polarization switching and domain-wall motion, including sluggish domain-wall motion, robust ferroelectricity in thin films, and the observation that the antipolar Pbca phase can hardly be transformed to the ferroelectric Pca21 phase by an electric field. Our mode analysis method can be more generally applied to any improper or hybrid improper ferroelectric, in which polarization switching requires changes of nonpolar distortions, for systematic and efficient prediction of optimal switching paths and estimation of coercive fields.

Original language	American English
Article number	134106
Journal	Physical Review B
Volume	111
Issue number	13
DOIs	https://doi.org/10.1103/PhysRevB.111.134106
State	Published - Apr 1 2025

ASJC Scopus subject areas

Electronic, Optical and Magnetic Materials
Condensed Matter Physics

Access to Document

10.1103/PhysRevB.111.134106

Cite this

@article{596c865f9fc04edca5de23ba2ad14ed0,

title = "Polarization switching in ferroelectric HfO2 from first-principles lattice mode analysis",

abstract = "In this paper, we introduce a first-principles-based lattice mode analysis method to investigate the competition between different polarization switching paths in HfO2. Because the stability of the polar orthorhombic Pca21 phase of HfO2 arises from a trilinear coupling, polarization switching requires the flipping of not only the polar Γ15Z mode, but also at least one zone-boundary antipolar mode. This means that each polarization state has multiple variants, leading to multiple possible switching paths connecting up- and down-polarized states, which can be systemically enumerated within this framework for efficient identification of the optimal switching path. Our lattice mode analysis also explains why the activation energy of propagation of the most widely studied domain-wall structure in HfO2, which requires the reversal of the X2- mode, is much larger than that of propagation of domain-wall structures with a uniform sign for the X2- mode. This approach deepens our understanding of distinctive properties of ferroelectric HfO2 related to polarization switching and domain-wall motion, including sluggish domain-wall motion, robust ferroelectricity in thin films, and the observation that the antipolar Pbca phase can hardly be transformed to the ferroelectric Pca21 phase by an electric field. Our mode analysis method can be more generally applied to any improper or hybrid improper ferroelectric, in which polarization switching requires changes of nonpolar distortions, for systematic and efficient prediction of optimal switching paths and estimation of coercive fields.",

author = "Yubo Qi and Sobhit Singh and Rabe, {Karin M.}",

note = "Publisher Copyright: {\textcopyright} 2025 American Physical Society.",

year = "2025",

month = apr,

day = "1",

doi = "10.1103/PhysRevB.111.134106",

language = "American English",

volume = "111",

journal = "Physical Review B",

issn = "2469-9950",

publisher = "American Physical Society",

number = "13",

}

TY - JOUR

T1 - Polarization switching in ferroelectric HfO2 from first-principles lattice mode analysis

AU - Qi, Yubo

AU - Singh, Sobhit

AU - Rabe, Karin M.

PY - 2025/4/1

Y1 - 2025/4/1

N2 - In this paper, we introduce a first-principles-based lattice mode analysis method to investigate the competition between different polarization switching paths in HfO2. Because the stability of the polar orthorhombic Pca21 phase of HfO2 arises from a trilinear coupling, polarization switching requires the flipping of not only the polar Γ15Z mode, but also at least one zone-boundary antipolar mode. This means that each polarization state has multiple variants, leading to multiple possible switching paths connecting up- and down-polarized states, which can be systemically enumerated within this framework for efficient identification of the optimal switching path. Our lattice mode analysis also explains why the activation energy of propagation of the most widely studied domain-wall structure in HfO2, which requires the reversal of the X2- mode, is much larger than that of propagation of domain-wall structures with a uniform sign for the X2- mode. This approach deepens our understanding of distinctive properties of ferroelectric HfO2 related to polarization switching and domain-wall motion, including sluggish domain-wall motion, robust ferroelectricity in thin films, and the observation that the antipolar Pbca phase can hardly be transformed to the ferroelectric Pca21 phase by an electric field. Our mode analysis method can be more generally applied to any improper or hybrid improper ferroelectric, in which polarization switching requires changes of nonpolar distortions, for systematic and efficient prediction of optimal switching paths and estimation of coercive fields.

AB - In this paper, we introduce a first-principles-based lattice mode analysis method to investigate the competition between different polarization switching paths in HfO2. Because the stability of the polar orthorhombic Pca21 phase of HfO2 arises from a trilinear coupling, polarization switching requires the flipping of not only the polar Γ15Z mode, but also at least one zone-boundary antipolar mode. This means that each polarization state has multiple variants, leading to multiple possible switching paths connecting up- and down-polarized states, which can be systemically enumerated within this framework for efficient identification of the optimal switching path. Our lattice mode analysis also explains why the activation energy of propagation of the most widely studied domain-wall structure in HfO2, which requires the reversal of the X2- mode, is much larger than that of propagation of domain-wall structures with a uniform sign for the X2- mode. This approach deepens our understanding of distinctive properties of ferroelectric HfO2 related to polarization switching and domain-wall motion, including sluggish domain-wall motion, robust ferroelectricity in thin films, and the observation that the antipolar Pbca phase can hardly be transformed to the ferroelectric Pca21 phase by an electric field. Our mode analysis method can be more generally applied to any improper or hybrid improper ferroelectric, in which polarization switching requires changes of nonpolar distortions, for systematic and efficient prediction of optimal switching paths and estimation of coercive fields.

UR - http://www.scopus.com/inward/record.url?scp=105002329095&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=105002329095&partnerID=8YFLogxK

U2 - 10.1103/PhysRevB.111.134106

DO - 10.1103/PhysRevB.111.134106

M3 - Article

SN - 2469-9950

VL - 111

JO - Physical Review B

JF - Physical Review B

IS - 13

M1 - 134106