Origin of large negative electrocaloric effect in antiferroelectric 
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Vales-Castro, Pablo; Faye, Romain; Vellvehı́, M.; Nouchokgwe, Youri; Perpiñà, X.; Caicedo, José Manuel; Jordà, X.; Roleder, Krystian; Kajewski, Dariusz; Pérez‐Tomás, Amador; Defaÿ, E.; Catalán, Gustau

doi:10.1103/physrevb.103.054112

Cited by 49 publications

(30 citation statements)

References 52 publications

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“…However, there is no splitting of the heat flow peak as reported in the ceramic PbZrO 3 . [ 58 ] This is due to the partially driven electric‐field‐induced phase transition, as evident by the unsaturated P – E loops in Figure 4a,b. Furthermore, Figure 6b shows the contour plots of the electric field dependence of dielectric permittivity (see representative curve in Figure 4b) at different temperatures.…”

Section: Resultsmentioning

confidence: 97%

Room‐Temperature Symmetric Giant Positive and Negative Electrocaloric Effect in PbMg_0.5W_0.5O₃ Antiferroelectric Ceramic

et al. 2021

Adv Funct Materials

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As an emerging solid‐state refrigeration technology with zero‐emission and high energy conversion efficiency, there is a compelling need for ferroelectric materials with giant electrocaloric effects (ECEs) at room temperature suitable for refrigeration applications. The complex perovskite antiferroelectric (AFE), PbMg0.5W0.5O3, containing non‐equivalent B‐site ions with a symmetric giant positive and negative ECE near room temperature is presented. At the Curie temperature of 36 °C, the first‐order AFE–paraelectric phase transition gives rise to a large enthalpy change of 3.92 J g−1, more than four times that of BaTiO3. This leads to a significant ECE under the influence of an electric field. The direct electrocaloric characterization shows that the adiabatic temperature change, ΔT, exhibits symmetric peaks with a giant positive maximum of 1.79 K (ΔS = 1.68 J kg−1 K−1) at 36 °C and a negative maximum of −2.02 K (ΔS = −1.93 J kg−1 K−1) at 34 °C. The ultrahigh magnitude of ΔT near room temperature makes PbMg0.5W0.5O3 a superior electrocaloric material far beyond traditional PbZrO3‐based AFEs. The coexistence of symmetric giant positive and negative ΔT to further improve cooling efficiency is expected. In addition, the good reversibility and negligible leakage current should pave the way for practical applications.

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Section: Resultsmentioning

confidence: 97%

Room‐Temperature Symmetric Giant Positive and Negative Electrocaloric Effect in PbMg_0.5W_0.5O₃ Antiferroelectric Ceramic

et al. 2021

Adv Funct Materials

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“…Although receiving less attention than FEs, AFE materials have been investigated for their intriguing physical properties, including the origin of antiferroelectricity [10][11][12][13], electromechanical coupling [14], electrocaloric effect [15][16][17] and negative capacitance [18]. In fact, AFE-based materials have been proposed to design memory devices [19,20].…”

Section: Introductionmentioning

confidence: 99%

“…Materials 2021, 14, x FOR PEER REVIEW Although receiving less attention than FEs, AFE materials have been inve their intriguing physical properties, including the origin of antiferroelectric electromechanical coupling [14], electrocaloric effect [15][16][17] and negative [18]. In fact, AFE-based materials have been proposed to design memory dev In recent years, both AFE-based and relaxor FE (RFE)-based capacitors [21][22][23][24][25][26] widely investigated due to their reducible energy loss [22,27], improvable polarization (Pmax), breakdown electric field (EB) [28][29][30] and energy efficiency Recently, a series of promising data have been reported [32][33][34][35][36].…”

Section: Introductionmentioning

confidence: 99%

Structural Phase Transition and In-Situ Energy Storage Pathway in Nonpolar Materials: A Review

2021

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Benefitting from exceptional energy storage performance, dielectric-based capacitors are playing increasingly important roles in advanced electronics and high-power electrical systems. Nevertheless, a series of unresolved structural puzzles represent obstacles to further improving the energy storage performance. Compared with ferroelectrics and linear dielectrics, antiferroelectric materials have unique advantages in unlocking these puzzles due to the inherent coupling of structural transitions with the energy storage process. In this review, we summarize the most recent studies about in-situ structural phase transitions in PbZrO3-based and NaNbO3-based systems. In the context of the ultrahigh energy storage density of SrTiO3-based capacitors, we highlight the necessity of extending the concept of antiferroelectric-to-ferroelectric (AFE-to-FE) transition to broader antiferrodistortive-to-ferrodistortive (AFD-to-FD) transition for materials that are simultaneously ferroelastic. Combining discussion of the factors driving ferroelectricity, electric-field-driven metal-to-insulator transition in a (La1−xSrx)MnO3 electrode is emphasized to determine the role of ionic migration in improving the storage performance. We believe that this review, aiming at depicting a clearer structure–property relationship, will be of benefit for researchers who wish to carry out cutting-edge structure and energy storage exploration.

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“…[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.…”

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confidence: 99%

“…The ability of antiferroelectrics 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 antiferroelectric 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].…”

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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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Origin of large negative electrocaloric effect in antiferroelectric PbZrO3

Cited by 49 publications

References 52 publications

Room‐Temperature Symmetric Giant Positive and Negative Electrocaloric Effect in PbMg_0.5W_0.5O₃ Antiferroelectric Ceramic

Room‐Temperature Symmetric Giant Positive and Negative Electrocaloric Effect in PbMg_0.5W_0.5O₃ Antiferroelectric Ceramic

Structural Phase Transition and In-Situ Energy Storage Pathway in Nonpolar Materials: A Review

Direct Visualization of Anti‐Ferroelectric Switching Dynamics via Electrocaloric Imaging

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Origin of large negative electrocaloric effect in antiferroelectric PbZrO3

Cited by 49 publications

References 52 publications

Room‐Temperature Symmetric Giant Positive and Negative Electrocaloric Effect in PbMg0.5W0.5O3 Antiferroelectric Ceramic

Room‐Temperature Symmetric Giant Positive and Negative Electrocaloric Effect in PbMg0.5W0.5O3 Antiferroelectric Ceramic

Structural Phase Transition and In-Situ Energy Storage Pathway in Nonpolar Materials: A Review

Direct Visualization of Anti‐Ferroelectric Switching Dynamics via Electrocaloric Imaging

Contact Info

Product

Resources

About

Room‐Temperature Symmetric Giant Positive and Negative Electrocaloric Effect in PbMg_0.5W_0.5O₃ Antiferroelectric Ceramic

Room‐Temperature Symmetric Giant Positive and Negative Electrocaloric Effect in PbMg_0.5W_0.5O₃ Antiferroelectric Ceramic