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<p>This study presents a strategy to enhance the pyroelectric and electrocaloric responses at room temperature by tailoring the Landau free-energy landscape of a ternary morphotropic phase boundary (MPB) composition 0.55Pb(Ni<sub>1/3</sub>Nb<sub>2/3</sub>)O<sub>3</sub>–0.135PbZrO<sub>3</sub>–0.315PbTiO<sub>3</sub> + <i>x</i>Eu<sub>2</sub>O<sub>3</sub> (<i>x</i> = 0, 0.01, and 0.02). Eu<sup>3+</sup> substitution at the A-site reduces the effective ionic spacing, inducing octahedral tilting and stabilizing a lower-symmetry crystal structure, predominantly rhombohedral, in the vicinity of room temperature. The associated local lattice distortion and charge imbalance promote relaxor behaviour in the PNN–PZ–PT system. A pronounced enhancement in pyroelectric performance is observed for the <i>x</i> = 0.02 composition, with the pyroelectric coefficient reaching ~ 33.34 × 10<sup>−4</sup>C/m<sup>2</sup>K and the corresponding pyroelectric figures of merit (FOMs) attaining values of <InlineEquation ID="IEq1"> <EquationSource Format="TEX">\({F}_{\text{i}}\)</EquationSource> <EquationSource Format="MATHML"><math> <msub> <mi>F</mi> <mtext>i</mtext> </msub> </math></EquationSource> </InlineEquation> ~ 1993&#xa0;pm/V, <InlineEquation ID="IEq2"> <EquationSource Format="TEX">\({F}_{\text{v}}\)</EquationSource> <EquationSource Format="MATHML"><math> <msub> <mi>F</mi> <mtext>v</mtext> </msub> </math></EquationSource> </InlineEquation> ~ 0.01592 m<sup>2</sup>/C, <InlineEquation ID="IEq3"> <EquationSource Format="TEX">\({F}_{\text{d}}\)</EquationSource> <EquationSource Format="MATHML"><math> <msub> <mi>F</mi> <mtext>d</mtext> </msub> </math></EquationSource> </InlineEquation> ~23.57 μ(Pa)<sup>−0.5</sup>, <InlineEquation ID="IEq4"> <EquationSource Format="TEX">\({F}_{\text{e}}\)</EquationSource> <EquationSource Format="MATHML"><math> <msub> <mi>F</mi> <mtext>e</mtext> </msub> </math></EquationSource> </InlineEquation> ~107 Jm<sup>3</sup>/K, and <InlineEquation ID="IEq5"> <EquationSource Format="TEX">\({F}_{\text{e}}^{*}\)</EquationSource> <EquationSource Format="MATHML"><math> <mmultiscripts> <mi>F</mi> <mrow> <mtext>e</mtext> </mrow> <mrow> <mrow /> <mo>∗</mo> </mrow> </mmultiscripts> </math></EquationSource> </InlineEquation> ~26.48 pm<sup>3</sup>/N. Notably, electrocaloric measurements reveal the emergence of an orthorhombic phase near room temperature, resulting in an improved electrocaloric temperature change. Concurrently, Eu<sup>3+</sup> doping suppresses the inverse piezoelectric coefficient (<InlineEquation ID="IEq6"> <EquationSource Format="TEX">\({d}_{33}^{*}\)</EquationSource> <EquationSource Format="MATHML"><math> <mmultiscripts> <mi>d</mi> <mrow> <mn>33</mn> </mrow> <mrow> <mrow /> <mo>∗</mo> </mrow> </mmultiscripts> </math></EquationSource> </InlineEquation>) from 1036&#xa0;pm/V for <i>x</i> = 0 to 460&#xa0;pm/V for <i>x</i> = 0.02 sample indicating reduced electromechanical coupling, while the energy storage density exhibits an improvement near the ferroelectric–paraelectric phase transition. These findings demonstrate that Eu<sup>3+−</sup> modified PNN–PZ–PT ceramics offer a tunable multifunctional platform with potential applications in solid-state cooling, infrared detection, and thermal energy harvesting.</p>

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Multifunctional pyroelectric and electrocaloric response through Eu3+ doping in 0.55Pb(Ni1/3Nb2/3)O3–0.135PbZrO3–0.315PbTiO3 ceramics at morphotropic phase boundary

  • 期刊论文

  • 发表日期：

    2026年4月8日

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  • Shubham Modgil,
  • Mukul Kumar,
  • Arun Kumar Singh,
  • Shobhna Dhiman,
  • Gyaneshwar Sharma,
  • O. P. Thakur,
  • Sanjeev Kumar

摘要

This study presents a strategy to enhance the pyroelectric and electrocaloric responses at room temperature by tailoring the Landau free-energy landscape of a ternary morphotropic phase boundary (MPB) composition 0.55Pb(Ni1/3Nb2/3)O3–0.135PbZrO3–0.315PbTiO3 + xEu2O3 (x = 0, 0.01, and 0.02). Eu3+ substitution at the A-site reduces the effective ionic spacing, inducing octahedral tilting and stabilizing a lower-symmetry crystal structure, predominantly rhombohedral, in the vicinity of room temperature. The associated local lattice distortion and charge imbalance promote relaxor behaviour in the PNN–PZ–PT system. A pronounced enhancement in pyroelectric performance is observed for the x = 0.02 composition, with the pyroelectric coefficient reaching ~ 33.34 × 10−4C/m2K and the corresponding pyroelectric figures of merit (FOMs) attaining values of \({F}_{\text{i}}\) F i ~ 1993 pm/V, \({F}_{\text{v}}\) F v ~ 0.01592 m2/C, \({F}_{\text{d}}\) F d ~23.57 μ(Pa)−0.5, \({F}_{\text{e}}\) F e ~107 Jm3/K, and \({F}_{\text{e}}^{*}\) F e ∗ ~26.48 pm3/N. Notably, electrocaloric measurements reveal the emergence of an orthorhombic phase near room temperature, resulting in an improved electrocaloric temperature change. Concurrently, Eu3+ doping suppresses the inverse piezoelectric coefficient ( \({d}_{33}^{*}\) d 33 ∗ ) from 1036 pm/V for x = 0 to 460 pm/V for x = 0.02 sample indicating reduced electromechanical coupling, while the energy storage density exhibits an improvement near the ferroelectric–paraelectric phase transition. These findings demonstrate that Eu3+− modified PNN–PZ–PT ceramics offer a tunable multifunctional platform with potential applications in solid-state cooling, infrared detection, and thermal energy harvesting.