Uncompensated Polarization in Incommensurate Modulations of Perovskite Antiferroelectrics

Ma, Tao; Fan, Z. Hugh; Xu, Bin; Kim, Tae Hoon; Lü, Ping; Bellaïche, L.; Kramer, M. J.; Tan, Xiaoli; Zhou, Lin

doi:10.1103/physrevlett.123.217602

Cited by 58 publications

(71 citation statements)

References 30 publications

(20 reference statements)

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“…The complex IMS was firstly investigated by MacLaren et al in (Pb 0.96 La 0.04 ) (Zr 0.9 Ti 0.1 ) 0.99 O 3 ceramics on atomic-scale, where the modulation of A-site cations was found to exist in a sinusoidal fashion 22 . Ma et al further pointed out that the A-site cations were either antiparallel but imbalanced or in a nearly orthogonal arrangement in (Pb 0.99 Nb 0.02 [(Zr 0.57 Sn 0.43 ) 1−y Ti y ] 0.98 O 3 ceramics 23 . These works have been regarded as an extraordinary step forward to the understanding of cation displacement in IMS.…”

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confidence: 99%

Unveiling the ferrielectric nature of PbZrO3-based antiferroelectric materials

Chen

et al. 2020

Nat Commun

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Benefitting from the reversible phase transition between antiferroelectric and ferroelectric states, antiferroelectric materials have recently received widespread attentions for energy storage applications. Antiferroelectric configuration with specific antiparallel dipoles has been used to establish antiferroelectric theories and understand its characteristic behaviors. Here, we report that the so-called antiferroelectric (Pb,La)(Zr,Sn,Ti)O 3 system is actually ferrielectric in nature. We demonstrate different ferrielectric configurations, which consists of ferroelectric ordering segments with either magnitude or angle modulation of dipoles. The ferrielectric configurations are mainly contributed from the coupling between A-cations and O-anions, and their displacement behavior is dependent largely on the chemical doping. Of particular significance is that the width and net polarization of ferroelectric ordering segments can be tailored by composition, which is linearly related to the key electrical characteristics, including switching field, remanent polarization and dielectric constant. These findings provide opportunities for comprehending structure-property correlation, developing antiferroelectric/ferrielectric theories and designing novel ferroic materials.

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confidence: 99%

Unveiling the ferrielectric nature of PbZrO3-based antiferroelectric materials

Chen

et al. 2020

Nat Commun

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“…This result is qualitatively consistent with Tan's HRTEM characterization in the same composition, which revealed the unbalanced cation displacements in the context of hierarchical domain structures. 220 Very recently, Fu et al also verified the "FE-like" dipole arrangement in PLZT using annular bright-field scanning transmission electron microscopy (STEM). 221…”

Section: Incommensurate Modulationmentioning

confidence: 98%

Antiferroelectrics: History, fundamentals, crystal chemistry, crystal structures, size effects, and applications

et al. 2021

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Antiferroelectric (AFE) materials are of great interest owing to their scientific richness and their utility in high-energy density capacitors. Here, the history of AFEs is reviewed, and the characteristics of antiferroelectricity and the phase transition of an AFE material are described. AFEs are energetically close to ferroelectric (FE) phases, and thus both the electric field strength and applied stress (pressure) influence the nature of the transition. With the comparable energetics between the AFE and FE phases, there can be a competition and frustration of these phases, and either incommensurate and/or a glassy (relaxor) structures may be observed. The phase transition in AFEs can also be influenced by the crystal/grain size, particularly at nanometric dimensions, and may be tuned through the formation of solid solutions. There have been extensive studies on the perovskite family of AFE materials, but many other crystal structures host AFE behavior, such as CuBiP 2 Se 6 . AFE applications include DC-link capacitors for power electronics, defibrillator capacitors, pulse power devices, and electromechanical actuators. The paper concludes with a perspective on the future needs and opportunities with respect to discovery, science, and applications of AFE. K E Y W O R D S applications, dielectric materials/properties, ferroelectricity/ferroelectric materials, phase transition F I G U R E 3 Antiferroelectric double hysteresis loops in (A) Pb(Lu 0.5 Nb 0.5 )O 3 and (B) the temperature-dependent critical field in it (replotted from Ref. [30]). (C) shows the phase diagram of PbZrO 3 as a function of temperature and electrical field (replotted from Ref.

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“…On the other hand, the small critical thickness (≈6.5 nm) provides a favorable condition for resolving the structural order parameters, [ 16,17 ] for example, tilting of oxygen octahedra, [ 18,19 ] and dynamically tracking their evolution during the AFE‐to‐FE transition. In addition, we find that the remnant polarization ( P r ), ranging from ≈2.5 to 8.3 µC cm −2 in the polarization–electric field ( P–E ) double‐hysteresis loop (Figure 1a and Figure S1, Supporting Information), is ubiquitous in pure and doped PbZrO 3 , [ 12,20–22 ] AgNbO 3 , and NaNbO 3 . [ 23–25 ] As a factor of reducing the U e , the inescapable P r , irrelevant to antiparallel cation shifts with either complete or partial offset, motivates us to find out its relationship with the ubiquitous structural defects, for example, point and planar defects.…”

Section: Introductionmentioning

confidence: 99%

In Situ Observation of Point‐Defect‐Induced Unit‐Cell‐Wise Energy Storage Pathway in Antiferroelectric PbZrO₃

Wei

Jia

Roleder

et al. 2021

Adv Funct Materials

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Phase transition is established to govern electrostatic energy storage for antiferroelectric (AFE)‐type dielectric capacitors. However, the source of inducing the phase transition and the pathway of storing the energy remains elusive so far given the ultrafast charging/discharging process under normal working conditions. Here, by slowing down the phase‐transition speed using electron‐beam irradiation as an external stimulus, the in situ dynamic energy‐storage process in AFE PbZrO3 is captured by using atomic‐resolution transmission electron microscopy. Specifically, it is found that oxygen‐lead‐vacancy‐induced defect core acts as a seed to initiate the antiferrodistortive‐to‐ferrodistortive transition in antiparallel‐Pb‐based structural frames. Associated with polarity evolution of the compressively strained defect core, the ferroelectric (FE)–ferrodistortive state expands bilaterally along the b‐axis direction and then develops into charged domain configurations during the energy‐storage process, which is further evidenced by observations at the ordinary FE states. With filling the gap of perception, the findings here provide a straightforward approach of unveiling the unit‐cell‐wise energy storage pathway in chemical defect‐engineered dielectric ceramics.

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Uncompensated Polarization in Incommensurate Modulations of Perovskite Antiferroelectrics

Cited by 58 publications

References 30 publications

Unveiling the ferrielectric nature of PbZrO3-based antiferroelectric materials

Unveiling the ferrielectric nature of PbZrO3-based antiferroelectric materials

Antiferroelectrics: History, fundamentals, crystal chemistry, crystal structures, size effects, and applications

In Situ Observation of Point‐Defect‐Induced Unit‐Cell‐Wise Energy Storage Pathway in Antiferroelectric PbZrO₃

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Uncompensated Polarization in Incommensurate Modulations of Perovskite Antiferroelectrics

Cited by 58 publications

References 30 publications

Unveiling the ferrielectric nature of PbZrO3-based antiferroelectric materials

Unveiling the ferrielectric nature of PbZrO3-based antiferroelectric materials

Antiferroelectrics: History, fundamentals, crystal chemistry, crystal structures, size effects, and applications

In Situ Observation of Point‐Defect‐Induced Unit‐Cell‐Wise Energy Storage Pathway in Antiferroelectric PbZrO3

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Product

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In Situ Observation of Point‐Defect‐Induced Unit‐Cell‐Wise Energy Storage Pathway in Antiferroelectric PbZrO₃