Giant electrocaloric effect at the antiferroelectric-to-ferroelectric phase boundary in Pb(Zr<i>x</i>Ti1–<i>x</i>)O3

Kimmel, Anna V.; Gindele, Oliver; Duffy, Dorothy M.; Cohen, R. E.

doi:10.1063/1.5096592

Cited by 20 publications

(17 citation statements)

References 25 publications

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“…1(b)] above the AFE-FE transition point (E < E AFE−FE ), its role is negligible compared to that of the latent heat of transformation. In addition, our maximum negative T matches atomistic calculations for the antiferroelectric-ferroelectric phase boundary [48], which is also consistent with a first-order phasetransition origin.…”

Section: Discussionsupporting

confidence: 86%

Origin of large negative electrocaloric effect in antiferroelectric PbZrO3

et al. 2021

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Section: Discussionsupporting

confidence: 86%

Origin of large negative electrocaloric effect in antiferroelectric PbZrO3

et al. 2021

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“…The samples examined in this study are ceramics of pure PZO, an archetypal anti-ferroelectric with a large negative electrocaloric effect. [5,27,28] Thanks to the electrocaloric temperature change concomitant with the AFE-FE phase transition (with Pbam [29] and R3c [30] symmetries, respectively), it is possible to use an infrared camera to observe how the electrocaloric front linked to the AFE switching nucleates/propagates across the sample in real time at a maximum frequency of 1253 Hz. In order to be able to switch the bulk ceramic capacitors with electric fields lower than the breakdown field, we work at temperatures close to, but below, the Curie temperature, which for PZO is T C ≈ 230 °C.…”

Section: Resultsmentioning

confidence: 99%

“…The samples examined in this study are ceramics of pure PbZrO 3 (PZO), an archetypal antiferroelectric with a large negative electrocaloric effect [5], [24], [25]. Thanks to the electrocaloric temperature change concomitant with the AFE-FE phase transition, it is possible to use an infrared camera to observe how the electrocaloric front linked to the AFE switching nucleates/propagates across the sample in real time at a maximum frequency of 1253 Hz.…”

mentioning

confidence: 99%

Direct Visualization of Anti‐Ferroelectric Switching Dynamics via Electrocaloric Imaging

Vales-Castro

Vellvehı́

Perpiñà

et al. 2021

Adv Elect Materials

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or even the standard gas cooling cycle (50%). [1] First theorized in 1878 by William Thomson, [2] the high-temperature changes (ΔT = 12 K) calculated for ferroelectric (FE) thin films [3] and the discovery of an anomalous electrocaloric effect in anti-ferroelectrics (AFE) [3] have renewed its interest, with an eye put on its potential application as a solid-state cooling solution in integrated circuits.FE materials display what is regarded as the "conventional" electrocaloric effect (or positive electrocaloric effect), whereby the material increases temperature (ΔT > 0) when a voltage step is applied and decreases temperature (ΔT < 0) when it is removed. In contrast, AFE display the opposite response; they decrease temperature (ΔT < 0) when an electric field E is applied, and increase (ΔT > 0) when it is removed. The ability of anti-ferroelectrics to cool down despite electrostatic energy being pumped into them is intriguing, and different underlying mechanisms have been proposed for the negative electrocaloric effect. [4,5] Recent experimental evidence indicates that, in the archetypal anti-ferroelectric PbZrO 3 (PZO), the so-called giant negative electrocaloric effect is due to the latent heat absorbed during the adiabatic-field-induced AFE-FE transition, which is endothermic. [6] In PbZrO 3 , the direct link between the anomalous electrocaloric effect and the first-order anti-ferroelectric-ferroelectric switching implies that the field-induced nucleation and motion of the AFE-FE phase boundary will dictate the dynamics of the large negative ECE and, ultimately, the dynamics of electrocaloric devices based on first-order transitions. In ferroelectrics, the study of domain wall dynamics [7][8][9][10][11][12][13][14][15][16] has been examined in detail on account of their relevance for ferroelectric memories. In contrast, there are far fewer works regarding the dynamics of the ferroelectric-paraelectric phase boundaries in FE [17,18] or the anti-ferroelectric-ferroelectric ones in anti-ferroelectrics. [19][20][21][22][23] Yet, a priori, one cannot assume that the dynamics of domain walls will be the same as the dynamics of phase boundaries, while the former separate different domains within the same ferroelectric phase, the latter separate different phases-in antiferroelectrics, an antipolar phase from a field-induced polar one. Domain switching dynamics is defined by a nucleationpropagation process. On the one hand, nucleation refers to the appearance of "hotspots," where nanoscopic nuclei of switched domains appear and rapidly expand forward across the thickness The large electrocaloric coupling in PbZrO 3 allows using high-speed infrared imaging for visualizing anti-ferroelectric switching dynamics via the associated temperature change. It is found that in ceramic samples of homogeneous temperature and thickness, switching is fast due to the generation of multiple nucleation sites, with devices responding in the millisecond range. By introducing gradients of thickness, however, it is possible to change the dyn...

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“…In contrast, AFE show a negative ECE, where the isothermal entropy change, ΔS, is positive (Figure 8B) and the adiabatic temperature change, ΔT, is negative under an increasing electric field. [53][54][55] The negative ECE sign in AFEs was suggested to originate from the dipole disruption by moderate field, but may also be associated with the phase transition sequence and the presence of commensurate/incommensurate ordering.…”

Section: Fe'smentioning

confidence: 99%

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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Giant electrocaloric effect at the antiferroelectric-to-ferroelectric phase boundary in Pb(ZrxTi1–x)O3

Cited by 20 publications

References 25 publications

Origin of large negative electrocaloric effect in antiferroelectric PbZrO3

Origin of large negative electrocaloric effect in antiferroelectric PbZrO3

Direct Visualization of Anti‐Ferroelectric Switching Dynamics via Electrocaloric Imaging

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

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