﻿<article xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">
  <front>
    <journal-meta>
      <journal-id journal-id-type="nlm-ta">Microstructures</journal-id>
      <journal-id journal-id-type="publisher-id">MICROSTRUCTURES</journal-id>
      <journal-title-group>
        <journal-title>Microstructures</journal-title>
      </journal-title-group>
      <issn pub-type="epub">2770-2995</issn>
      <publisher>
        <publisher-name>OAE Publishing Inc.</publisher-name>
      </publisher>
    </journal-meta>
    <article-meta>
      <article-id pub-id-type="doi">10.20517/microstructures.2026.93</article-id>
      <article-categories>
        <subj-group>
          <subject>Research Article</subject>
        </subj-group>
      </article-categories>
      <title-group>
        <article-title>Incommensurate modulations and thickness-dependent energy storage density in (PbLaSrBa)(ZrSnTi)O<sub>3</sub> relaxor antiferroelectric thick-film ceramics</article-title>
      </title-group>
      <contrib-group>
        <contrib contrib-type="author" corresp="yes">
          <name>
            <surname>Lu</surname>
            <given-names>Sheng-Guo</given-names>
          </name>
          <xref ref-type="aff" rid="I1">
            <sup>1</sup>
          </xref>
          <xref ref-type="corresp" rid="cor1" />
          <contrib-id contrib-id-type="orcid">https://orcid.org/0000-0001-9555-656X</contrib-id>
        </contrib>
        <contrib contrib-type="author">
          <name>
            <surname>Yan</surname>
            <given-names>Xuling</given-names>
          </name>
          <xref ref-type="aff" rid="I1">
            <sup>1</sup>
          </xref>
        </contrib>
        <contrib contrib-type="author" corresp="yes">
          <name>
            <surname>Gao</surname>
            <given-names>Xiaoyi</given-names>
          </name>
          <xref ref-type="aff" rid="I2">
            <sup>2</sup>
          </xref>
          <xref ref-type="corresp" rid="cor1" />
        </contrib>
        <contrib contrib-type="author">
          <name>
            <surname>Yu</surname>
            <given-names>Chao</given-names>
          </name>
          <xref ref-type="aff" rid="I1">
            <sup>1</sup>
          </xref>
        </contrib>
        <contrib contrib-type="author">
          <name>
            <surname>Li</surname>
            <given-names>Yuxuan</given-names>
          </name>
          <xref ref-type="aff" rid="I1">
            <sup>1</sup>
          </xref>
        </contrib>
        <contrib contrib-type="author" corresp="yes">
          <name>
            <surname>Wang</surname>
            <given-names>Shibin</given-names>
          </name>
          <xref ref-type="aff" rid="I1">
            <sup>1</sup>
          </xref>
          <xref ref-type="corresp" rid="cor1" />
        </contrib>
        <contrib contrib-type="author">
          <name>
            <surname>Yao</surname>
            <given-names>Yingbang</given-names>
          </name>
          <xref ref-type="aff" rid="I1">
            <sup>1</sup>
          </xref>
        </contrib>
        <contrib contrib-type="author">
          <name>
            <surname>Tao</surname>
            <given-names>Tao</given-names>
          </name>
          <xref ref-type="aff" rid="I1">
            <sup>1</sup>
          </xref>
        </contrib>
        <contrib contrib-type="author">
          <name>
            <surname>Liang</surname>
            <given-names>Bo</given-names>
          </name>
          <xref ref-type="aff" rid="I1">
            <sup>1</sup>
          </xref>
        </contrib>
        <contrib contrib-type="author">
          <name>
            <surname>Gong</surname>
            <given-names>Weiping</given-names>
          </name>
          <xref ref-type="aff" rid="I3">
            <sup>3</sup>
          </xref>
        </contrib>
        <contrib contrib-type="author" corresp="yes">
          <name>
            <surname>Niu</surname>
            <given-names>Xiang</given-names>
          </name>
          <xref ref-type="aff" rid="I1">
            <sup>1</sup>
          </xref>
          <xref ref-type="corresp" rid="cor1" />
        </contrib>
        <contrib contrib-type="author" corresp="yes">
          <name>
            <surname>Jian</surname>
            <given-names>Xiaodong</given-names>
          </name>
          <xref ref-type="aff" rid="I1">
            <sup>1</sup>
          </xref>
          <xref ref-type="aff" rid="I4">
            <sup>4</sup>
          </xref>
          <xref ref-type="corresp" rid="cor1" />
        </contrib>
      </contrib-group>
      <aff id="I1">
        <sup>1</sup>State Key Laboratory of Precision Electronic Manufacturing Technology and Equipment, Guangdong Provincial Research Center on Smart Materials and Energy Conversion Devices, School of Materials and Energy, School of Electromechanical Engineering and School of Integrated Circuits, Guangdong University of Technology, Guangzhou 510006, Guangdong, China.</aff>
      <aff id="I2">
        <sup>2</sup>Shandong Provincial Key Laboratory of High-Performance Ceramics and Precision Manufacturing, Shandong Industrial Ceramics Research and Design Institute Co., Ltd, Zibo 255000, Shandong, China.</aff>
      <aff id="I3">
        <sup>3</sup>Guangdong Provincial Key Laboratory of Electronic Functional Materials and Devices, Huizhou University, Huizhou 516001, Guangdong, China.</aff>
      <aff id="I4">
        <sup>4</sup>Science and Technology on Reliability Physics and Application of Electronic Component Laboratory, The 5th Electronics Research Institute of the Ministry of Industry and Information Technology, Guangzhou 510610, Guangdong, China.</aff>
      <author-notes>
        <corresp id="cor1">Correspondence to: Prof. Sheng-Guo Lu, Dr. Shibin Wang, Dr. Xiang Niu, State Key Laboratory of Precision Electronic Manufacturing Technology and Equipment, Guangdong Provincial Research Center on Smart Materials and Energy Conversion Devices, School of Materials and Energy, School of Electromechanical Engineering and School of Integrated Circuits, Guangdong University of Technology, Guangzhou 510006, Guangdong, China. E-mail: <email>sglu@gdut.edu.cn</email>; <email>shibinwang@gdut.edu.cn</email>; <email>Xiang.Niu@gdut.edu.cn</email>; Dr. Xiaoyi Gao, Shandong Provincial Key Laboratory of High-Performance Ceramics and Precision Manufacturing, Shandong Industrial Ceramics Research and Design Institute Co., Ltd, Zibo 255000, Shandong, China. E-mail: <email>xygao@whut.edu.cn</email>; Dr. Xiaodong Jian, State Key Laboratory of Precision Electronic Manufacturing Technology and Equipment, Guangdong Provincial Research Center on Smart Materials and Energy Conversion Devices, School of Materials and Energy, School of Electromechanical Engineering and School of Integrated Circuits, Guangdong University of Technology, Guangzhou 510006, Guangdong, China; Science and Technology on Reliability Physics and Application of Electronic Component Laboratory, The 5th Electronics Research Institute of the Ministry of Industry and Information Technology, Guangzhou 510610, Guangdong, China. E-mail: <email>jianxiaodong_gdut@126.com</email>.</corresp>
        <fn fn-type="other">
          <p>
            <bold>Received:</bold> 4 May 2026 |  <bold>First Decision:</bold> 2 Jun 2026 |  <bold>Revised:</bold> 14 Aug 2026 |  <bold>Accepted:</bold> 26 Aug 2026 |  <bold>Published:</bold> 28 Oct 2026</p>
        </fn>
        <fn fn-type="other">
          <p>
            <bold>Academic Editor:</bold> Dae-Yong Jeong | <bold>Copy Editor:</bold> Ping Zhang |  <bold>Production Editor:</bold> Ping Zhang</p>
        </fn>
      </author-notes>
	  <pub-date pub-type="ppub">
        <year>2026</year>
      </pub-date>
      <pub-date pub-type="epub">
        <day>28</day>
        <month>10</month>
        <year>2026</year>
      </pub-date>
      <volume>6</volume>
	  <issue>6</issue>
      <elocation-id>20260135</elocation-id>
      <permissions>
        <copyright-statement>© The Author(s) 2026.</copyright-statement>
        <license xlink:href="https://creativecommons.org/licenses/by/4.0/">
          <license-p>© The Author(s) 2026. <bold>Open Access</bold> This article is licensed under a Creative Commons Attribution 4.0 International License (<uri xlink:href="https://creativecommons.org/licenses/by/4.0/">https://creativecommons.org/licenses/by/4.0/</uri>), which permits unrestricted use, sharing, adaptation, distribution and reproduction in any medium or format, for any purpose, even commercially, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made.</license-p>
        </license>
      </permissions>
      <abstract>
        <p>In this study, (Pb<sub>0.92-x</sub>La<sub>0.04</sub>Sr<sub>x</sub>Ba<sub>0.02</sub>)(Zr<sub>0.64</sub>Sn<sub>0.35</sub>Ti<sub>0.01</sub>)O<sub>3</sub> (PLSBZSTi, i = 1 (x=0.04), 2 (0.06), 3 (0.08), and 4 (0.10)) relaxor antiferroelectric thick-film ceramics were prepared using a tape-casting process. An ultrahigh <italic>W<sub>rec</sub></italic> of 20.09 J/cm<sup>3</sup> with an ultrahigh <italic>η</italic> of 91.34% was obtained for the PLSBZST2 (x = 0.06) ceramic. This outstanding energy storage performance is attributed to the distinct microstructural features of this system. Specifically, transmission electron microscopy revealed the presence of nanosized stripe domains, along with F-spots associated with 1/2{ooo} superlattice diffraction and an incommensurate modulation structure (IMS) related to the 1/n&lt;110&gt; superlattice (n = 4.91). These microstructural characteristics are direct evidence of oxygen octahedral tilting, which promotes the formation of relatively slim hysteresis loops. Moreover, the inverse power-law relationship between the sample thickness and energy storage density was determined. The fitted exponent was -0.43 ± 0.04, which can be quantified by combining the thickness-dependent dielectric breakdown strength (exponent of -0.39) and maximum polarization (exponent of -0.13) with a 20% correction factor accounting for the practical underutilization of the maximum electric field and polarization.</p>
      </abstract>
      <kwd-group>
        <kwd>(PbLaSrBa)(ZrSnTi)O<sub>3</sub></kwd>
        <kwd>antiferroelectrics</kwd>
        <kwd>thick-film ceramics</kwd>
        <kwd>energy storage performance</kwd>
        <kwd>energy storage density versus thickness</kwd>
      </kwd-group>
    </article-meta>
  </front>
  <body>
    <sec id="sec1">
      <title>INTRODUCTION</title>
      <p>Compared with traditional lithium-ion batteries, electrochemical capacitors, and polymer media, ceramic-based dielectric capacitors offer high power densities and are attractive for meeting the growing demand for energy storage devices<sup>[<xref ref-type="bibr" rid="B1">1</xref>-<xref ref-type="bibr" rid="B5">5</xref>]</sup>, and many studies have attempted to develop these systems<sup>[<xref ref-type="bibr" rid="B6">6</xref>-<xref ref-type="bibr" rid="B10">10</xref>]</sup>. Ceramic-based dielectric capacitors have attracted much attention because of their high power densities, fast charge-discharge abilities, broad operating-temperature ranges, long cyclic times, and excellent thermal stabilities in pulse-power devices<sup>[<xref ref-type="bibr" rid="B11">11</xref>-<xref ref-type="bibr" rid="B16">16</xref>]</sup>. These characteristics make ceramic dielectric capacitors promising for energy storage applications such as pulse-power supplies, electric vehicles, and electromagnetic pulse devices<sup>[<xref ref-type="bibr" rid="B17">17</xref>-<xref ref-type="bibr" rid="B19">19</xref>]</sup>.</p>
      <p>Dielectric materials can be classified into four categories: linear dielectrics, normal ferroelectrics, antiferroelectrics (AFEs), and relaxor ferroelectrics<sup>[<xref ref-type="bibr" rid="B20">20</xref>-<xref ref-type="bibr" rid="B23">23</xref>]</sup>. Among them, AFEs show unique double polarization-electric field (P-E) hysteresis loops in an external electric field, experience a transition from an AFE phase to a ferroelectric (FE) phase with an increasing electric field, and demonstrate a transition from an FE to AFE phase in a decreasing electric field. Because of the antiparallel arrangement of adjacent dipoles, the remnant polarization of AFEs is near zero, and the polarization and dielectric constant sharply increase when the electric field reaches the transition field. These features improve the discharged energy storage density and charge-discharge performance of AFEs in terms of increasing the integrated area of the upper branch of P-E hysteresis loop with respect to the polarization axis<sup>[<xref ref-type="bibr" rid="B24">24</xref>-<xref ref-type="bibr" rid="B27">27</xref>]</sup>. The total energy storage density (<italic>W<sub>tot</sub></italic>), recoverable energy storage density (<italic>W<sub>rec</sub></italic>), and energy storage efficiency (<italic>η</italic>) of dielectric ceramic capacitors can be defined as follows<sup>[<xref ref-type="bibr" rid="B28">28</xref>,<xref ref-type="bibr" rid="B29">29</xref>]</sup>:</p>
      <p><disp-formula> <label>(1)</label> <tex-math id="E1"> $$ W_{t o t}=\int_{0}^{P_{m}} E d P  $$ </tex-math></disp-formula></p>
      <p><disp-formula> <label>(2)</label> <tex-math id="E2"> $$ W_{r e c}=\int_{P_{r}}^{P_{m}} E d P $$ </tex-math></disp-formula></p>
      <p><disp-formula> <label>(3)</label> <tex-math id="E3"> $$ \eta=\frac{W_{r e c}}{W_{t o t}} \times 100 \% $$ </tex-math></disp-formula></p>
      <p>where <italic>E</italic>, <italic>P<sub>m</sub></italic>, and <italic>P<sub>r</sub></italic> denote the applied electric field, maximum polarization, and remnant polarization, respectively.</p>
      <p>Therefore, improving the polarization, AFE-FE transition field, and dielectric breakdown strength (DBS) of AFE materials can enhance the energy storage performance of dielectric capacitors. The stability of the AFE phase can be evaluated using the Goldschmidt tolerance factor for the ABO<sub>3</sub> perovskite structure:</p>
      <p><disp-formula> <label>(4)</label> <tex-math id="E4"> $$ t=\frac{R_{A}+R_{O}}{\sqrt{2}\left(R_{B}+R_{O}\right)} $$ </tex-math></disp-formula></p>
      <p>where <italic>R<sub>A</sub></italic>, <italic>R<sub>B</sub></italic>, and <italic>R<sub>O</sub></italic> denote the radii of A-site, B-site, and oxygen ions, respectively. When ionic doping decreases t, the stability of the AFE phase increases, thus increasing the phase transition field E<sub>AFE-FE</sub>. For linear ferroelectrics, the polarization is usually proportional to the dielectric constant multiplied by the electric field, and it therefore increases with increasing electric field intensity. The DBS can be increased either intrinsically by increasing the bandgap through doping or extrinsically by refining the grain-size distribution to reduce defect concentration and interfacial flaws<sup>[<xref ref-type="bibr" rid="B30">30</xref>-<xref ref-type="bibr" rid="B32">32</xref>]</sup>. Liu <italic>et al.</italic><sup>[<xref ref-type="bibr" rid="B32">32</xref>,<xref ref-type="bibr" rid="B33">33</xref>]</sup> investigated (Pb<sub>0.925</sub>La<sub>0.05</sub>)(Zr<sub>0.995</sub>Ti<sub>0.005</sub>)O<sub>3</sub> ceramics and obtained <italic>W<sub>rec</sub></italic> = 12.3 J/cm<sup>3</sup> and <italic>η</italic> = 84% under an electric field of <InlineParagraph>420 kV/cm</InlineParagraph> by refining the grain size distribution and enhancing the bandgap (<inline-formula><tex-math id="M1">$$  E_{B} \propto e^{\sqrt{E_{g}}}  $$</tex-math></inline-formula>), where <italic>E<sub>B</sub></italic> is the DBS and <italic>E<sub>g</sub></italic> is the bandgap). Liu <italic>et al.</italic><sup>[<xref ref-type="bibr" rid="B31">31</xref>]</sup> also prepared a multilayer ceramic capacitor (Pb<sub>0.94</sub>La<sub>0.02</sub>Ca<sub>0.04</sub>)(Zr<sub>0.7</sub>Sn<sub>0.3</sub>)<sub>0.995</sub>O<sub>3</sub> via grain refinement and strengthened cation-O bonding, obtaining <italic>W<sub>rec</sub></italic> = 14.3 J/cm<sup>3</sup> and <italic>η</italic> = 86.1% at <InlineParagraph>530 kV/cm.</InlineParagraph> In addition, Li <italic>et al.</italic><sup>[<xref ref-type="bibr" rid="B34">34</xref>]</sup> investigated (Pb<sub>0.92</sub>Gd<sub>0.02</sub>Sr<sub>0.05</sub>)(Zr<sub>0.87</sub>Sn<sub>0.12</sub>Ti<sub>0.01</sub>)O<sub>3</sub> ceramics and achieved <italic>W<sub>rec</sub></italic> = 14.5 J/cm<sup>3</sup> and <italic>η</italic> = 81% at 717 kV/cm using a phase tailoring strategy via chemical modification.</p>
      <p>These previous studies found that although these materials demonstrate high energy-storage densities, their energy storage efficiencies remain relatively low. By contrast, the energy storage efficiency of (PbLa)(ZrSnTi)O<sub>3</sub> (PLZST) ceramics is related to the hysteresis of the AFE-FE and FE-AFE phase transitions. Previous investigations have shown that the electric hysteresis in the P-E loop can be reduced by doping Sr<sup>2+</sup> ions at A-sites, and a relaxor AFE with a diffuse phase transition can be constructed to form a slim P-E hysteresis loop, thereby effectively improving the energy storage efficiency of this system<sup>[<xref ref-type="bibr" rid="B11">11</xref>,<xref ref-type="bibr" rid="B35">35</xref>]</sup>. Moreover, the doping of Ba<sup>2+</sup> ions at A-sites has been shown to increase the dielectric constant and correspondingly decrease the phase transition temperature<sup>[<xref ref-type="bibr" rid="B36">36</xref>,<xref ref-type="bibr" rid="B37">37</xref>]</sup>. Therefore, this study investigated Ba<sup>2+</sup> and Sr<sup>2+</sup> co-doped PLZST AFE bulk ceramics. In addition, doped PLZST thick-film ceramics were fabricated using a tape-casting process to further improve the DBS and energy storage performance<sup>[<xref ref-type="bibr" rid="B38">38</xref>]</sup>. The effect of film thickness on DBS and polarization was evaluated, and the influence of the ceramic thickness on the energy storage density was statistically determined.</p>
    </sec>
    <sec id="sec2">
      <title>EXPERIMENTAL</title>
      <sec id="sec2-1">
        <title>Experimental methods</title>
        <p>First, (Pb<sub>0.92-x</sub>La<sub>0.04</sub>Sr<sub>x</sub>Ba<sub>0.02</sub>)(Zr<sub>0.64</sub>Sn<sub>0.35</sub>Ti<sub>0.01</sub>)O<sub>3</sub> (where x = 0.04, 0.06, 0.08, and 0.10; abbreviated as PLSBZST1, PLSBZST2, PLSBZST3, and PLSBZST4, respectively) ceramics were prepared using a tape-casting approach. Raw materials were purchased from Aladdin (China), including PbO (99.90%), La<sub>2</sub>O<sub>3</sub> (99.90%), SrCO<sub>3</sub> (99.00%), BaCO<sub>3</sub> (99.95%), ZrO<sub>2</sub> (99.99%), SnO<sub>2</sub> (99.50%), and TiO<sub>2</sub> (99.00%). The raw materials were weighed according to their stoichiometric ratios, and an excess of 3% PbO was added to compensate for PbO volatilization during high-temperature sintering. The mixture was ball milled (MSK-SFM-1, Kejing, China) at 250 rpm for 24 h using anhydrous ethanol as a solvent, dried at 100 °C overnight after ball milling, and the resulting green powders were calcined at 900 °C for 2 h. A second ball milling and drying step was then performed to obtain crystalline PLSBZST powders. Next, the PLSBZST ceramic powders were dispersed in a solvent. The dispersant, binder, and plasticizer were then added to prepare the slurry, which was tape-cast into PLSBZST thick-film green sheets. Finally, the thick-film green sheets were cut and debindered at 650 °C for 6 h, followed by sintering at 1,100~1,200 °C for 6 h to obtain dense, freestanding thick-film ceramics.</p>
      </sec>
      <sec id="sec2-2">
        <title>Microstructural characterization and performance testing</title>
        <p>The lattice structure was characterized using X-ray diffractometry (XRD; Rigaku, Ultima-Ⅳ). Rietveld refinement was carried out using FullProf software. The surface morphologies and elemental distributions of the ceramics were analyzed using scanning electron microscopy (SEM; S3400-N and SU8010, Hitachi High-Technologies Corporation, Japan) equipped with an energy-dispersive X-ray spectrometer (EDS). The grain size distribution was statistically analyzed using ImageJ software. Selected-area electron diffraction (SAED) patterns and high-resolution transmission electron microscopy (HRTEM) images were obtained using a Talos F200x microscope (FEI Company, USA). The temperature- and frequency-dependent dielectric constant and loss tangent were measured using a precision inductor-capacitor-resistor (LCR) analyzer (4980A, Keysight, USA). The P-E hysteresis loops of the ceramics were measured using a Sawyer-Tower circuit (Precision Multiferroic II ferroelectric test system, Radiant Technologies Inc., USA). Circular gold electrodes with a diameter of 1 mm were used for the P-E and other electrical measurements, whereas electrodes with a diameter of 1.8 mm were used for the charge-discharge measurements.</p>
      </sec>
    </sec>
    <sec id="sec3">
      <title>RESULTS AND DISCUSSION</title>
      <p>
        <xref ref-type="fig" rid="fig1">Figure 1A</xref> shows the XRD patterns of the PLSBZST1-4 AFE ceramics at room temperature. All ceramics demonstrate pure perovskite structures, and no diffraction peaks from the impurity phase are detected. In the magnified patterns near 2<italic>θ</italic> = 44°, the intensity of the (200) peak is approximately twice that of the (002) peak, indicating that the PLSBZST ceramics may have an orthorhombic structure<sup>[<xref ref-type="bibr" rid="B30">30</xref>,<xref ref-type="bibr" rid="B39">39</xref>,<xref ref-type="bibr" rid="B40">40</xref>]</sup>. According to the Bragg equation,</p>
      <fig id="fig1" position="float" width="450">
        <label>Figure 1</label>
        <caption>
          <p>(A1) XRD patterns obtained at room temperature for the PLSBZST thick-film ceramics; (A2) Magnified XRD patterns for 2θ ranging from 42° to 46°; and Rietveld refinements for (Pb<sub>0.92-x</sub>La<sub>0.04</sub>Sr<sub>x</sub>Ba<sub>0.02</sub>)(Zr<sub>0.64</sub>Sn<sub>0.35</sub>Ti<sub>0.01</sub>)O<sub>3</sub> thick-film ceramics with different x values: (B) x = 0.04, (C) x = 0.06, (D) x = 0.08, (E) x = 0.10. XRD: X-ray diffraction; PLSBZST: (Pb<sub>0.92-x</sub>La<sub>0.04</sub>Sr<sub>x</sub>Ba<sub>0.02</sub>)(Zr<sub>0.64</sub>Sn<sub>0.35</sub>Ti<sub>0.01</sub>)O<sub>3</sub>.</p>
        </caption>
        <graphic xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="microstructures6093.fig.1.jpg" />
      </fig>
      <p><disp-formula> <label>(5)</label> <tex-math id="E5"> $$ 2 d sin \theta=n \lambda $$ </tex-math></disp-formula></p>
      <p>where <italic>d</italic> is the distance between the two close crystalline planes, <italic>θ</italic> is the angle of incidence or the angle of reflection, <italic>n</italic> is the whole number, and <italic>λ</italic> is the wavelength of X-ray. The lattice shrinks and the lattice constant decreases as Sr<sup>2+</sup> (1.19 Å) has a smaller ionic radius than Pb<sup>2+</sup> (1.49 Å). Therefore, the diffraction peaks shift toward higher diffraction angles.</p>
      <p>Rietveld refinements were used to confirm the exact phase structures and detailed lattice parameters of all samples. <xref ref-type="fig" rid="fig1">Figure 1B</xref>-<xref ref-type="fig" rid="fig1">E</xref> demonstrates the Rietveld refinement results of the PLSBZST thick-film ceramics, which show that all thick-film ceramics adopt an orthorhombic phase structure (<italic>Pbam</italic> space group). <xref ref-type="table" rid="t1">Table 1</xref> summarizes the lattice parameters and reasonable agreement indices (<italic>R<sub>p</sub></italic>, <italic>R<sub>wp</sub></italic>, and <italic>χ</italic><sup>2</sup>).</p>
      <table-wrap id="t1">
        <label>Table 1</label>
        <caption>
          <p>Lattice parameters obtained using Rietveld refinement</p>
        </caption>
        <table frame="hsides" rules="groups">
          <thead>
            <tr>
              <td rowspan="2" style="border-bottom:1;">
                <bold>Composition</bold>
              </td>
              <td colspan="4" style="border-bottom:1;">
                <bold>Lattice parameters</bold>
              </td>
              <td rowspan="2" style="border-bottom:1;">
                <bold>Phase</bold>
              </td>
              <td rowspan="2" style="border-bottom:1;">
                <bold>R<sub>p</sub> (%)</bold>
              </td>
              <td rowspan="2" style="border-bottom:1;">    <bold>R<sub>wp</sub> (%)</bold></td>
              <td rowspan="2" style="border-bottom:1;">    <bold><italic>χ</italic><sup>2</sup></bold></td>
            </tr>
            <tr>
              <td style="border-bottom:1;">
                <bold>a (Å)</bold>
              </td>
              <td style="border-bottom:1;">
                <bold>b (Å)</bold>
              </td>
              <td style="border-bottom:1;">
                <bold>c (Å)</bold>
              </td>
              <td style="border-bottom:1;">
                <bold>Α = β = γ (°)</bold>
              </td>
            </tr>
          </thead>
          <tbody>
            <tr>
              <td>x = 0.04</td>
              <td>5.82617</td>
              <td>11.63645</td>
              <td>8.18836</td>
              <td>90</td>
              <td>O</td>
              <td>4.03</td>
              <td>5.32</td>
              <td>2.44</td>
            </tr>
            <tr>
              <td>x = 0.06</td>
              <td>5.82586</td>
              <td>11.63240</td>
              <td>8.18749</td>
              <td>90</td>
              <td>O</td>
              <td>3.65</td>
              <td>4.87</td>
              <td>2.37</td>
            </tr>
            <tr>
              <td>x = 0.08</td>
              <td>5.82329</td>
              <td>11.62583</td>
              <td>8.18616</td>
              <td>90</td>
              <td>O</td>
              <td>4.02</td>
              <td>5.25</td>
              <td>2.04</td>
            </tr>
            <tr>
              <td>x = 0.10</td>
              <td>5.82280</td>
              <td>11.62437</td>
              <td>8.18529</td>
              <td>90</td>
              <td>O</td>
              <td>3.70</td>
              <td>4.74</td>
              <td>2.94</td>
            </tr>
          </tbody>
        </table>
        <table-wrap-foot>
          <fn>
            <p>R<sub>p</sub>: Patterns; R<sub>wp</sub>: weighted patterns.</p>
          </fn>
        </table-wrap-foot>
      </table-wrap>
      <p>To further characterize the microstructures of PLSBZST ceramics, the sample with x = 0.06 was analyzed using transmission electron microscopy (TEM). In <xref ref-type="fig" rid="fig2">Figure 2A</xref>, typical nanosized stripe electric domains (e.g., ~200-300 nm in size) can be observed in the bright-field image. An HRTEM image covering an electric domain area with tens of nanometers in size is also shown in the inset of <xref ref-type="fig" rid="fig2">Figure 2A</xref>. The reduction in the size of the ordered regions is attributed to the disruption of long-range order caused by compositional and structural fluctuations. These nanosized domains, also called polar nanoregions (PNRs), result in slim P-E hysteresis loops and other typical relaxor AFE behaviors, such as diffuse phase transitions<sup>[<xref ref-type="bibr" rid="B11">11</xref>,<xref ref-type="bibr" rid="B35">35</xref>]</sup>. Moreover, the relaxor AFE diffuseness parameter is &gt; 1 and close to 1.6 (see <xref ref-type="fig" rid="fig2">Figure 2A</xref>)<sup>[<xref ref-type="bibr" rid="B41">41</xref>,<xref ref-type="bibr" rid="B42">42</xref>]</sup>. <xref ref-type="fig" rid="fig2">Figure 2B</xref> shows the SAED pattern obtained along the [<inline-formula><tex-math id="M2">$$  0\bar{1}1 $$</tex-math></inline-formula>] zone axis. In addition to the main reflection spots, 1/2{ooo}-type superlattice diffraction patterns (F-spots) are observed and indicated by the red boxes in <xref ref-type="fig" rid="fig2">Figure 2B</xref>. These reflections arise from the tilting of the oxygen octahedra within the crystalline structure. In <xref ref-type="fig" rid="fig2">Figure 2C</xref> and <xref ref-type="fig" rid="fig2">2D</xref>, the diffraction spots indicated by the hollow triangles are adjacent to the main diffraction spots, which may result from the incommensurate modulation structure (IMS) caused by the antiparallel displacement of cations<sup>[<xref ref-type="bibr" rid="B43">43</xref>,<xref ref-type="bibr" rid="B44">44</xref>]</sup>. As shown in <xref ref-type="fig" rid="fig2">Figure 2C</xref>, the IMS is formed along the <inline-formula><tex-math id="M3">$$  &lt;\bar{1}0\bar{1}&gt;  $$</tex-math></inline-formula> direction. The plane spacing (<inline-formula><tex-math id="M4">$$  d_{\bar{1}0\bar{1}} $$</tex-math></inline-formula>) results from an irrational number multiplied by the modulation wavelength in the diffraction spacing (<italic>λ</italic>) (i.e., <inline-formula><tex-math id="M5">$$  d_{\bar{1}0\bar{1}} $$</tex-math></inline-formula> = <italic>nλ</italic>, where <italic>n</italic> = 4.91)<sup>[<xref ref-type="bibr" rid="B43">43</xref>]</sup>. <xref ref-type="fig" rid="fig2">Figure 2D</xref> shows the SAED patterns obtained in the [010] direction near the 90° domain wall. The satellite patterns caused by the IMS are highlighted by the green and yellow hollow triangles, and these reflection patterns are arranged vertically along the &lt;101&gt; and <inline-formula><tex-math id="M6">$$  &lt;\bar{1}01 $$</tex-math></inline-formula> directions<sup>[<xref ref-type="bibr" rid="B44">44</xref>]</sup>. The existence of the IMS can produce a relatively slimmer hysteresis loop. For the relaxor AFE with an IMS structure, the shape of the hysteresis loop is slimmer and more inclined, which improves the energy storage density and efficiency of this system.</p>
      <fig id="fig2" position="float" width="550">
        <label>Figure 2</label>
        <caption>
          <p>TEM image and diffraction patterns for PLSBZST2 (x = 0.06) AFE thick-film ceramics. (A) Bright-field images of the stripe domains, and the inset shows an HRTEM image of a nanosized domain; (B) SAED pattern with 1/2{ooo} superlattice patterns (F-spots); (C) [<inline-formula><tex-math id="M9">$$ 0\bar{1}0 $$</tex-math></inline-formula>] SAED pattern showing the incommensurate modulation structure (IMS) in an AFE domain; (D) [010] SAED pattern demonstrating the IMS near the 90° domain wall. TEM: Transmission electron microscopy; AFE: antiferroelectric; PLSBZST2: (Pb<sub>0.86</sub>La<sub>0.04</sub>Sr<sub>0.06</sub>Ba<sub>0.02</sub>)(Zr<sub>0.64</sub>Sn<sub>0.35</sub>Ti<sub>0.01</sub>)O<sub>3</sub>; SAED: selected area electron diffraction; HRTEM: high resolution transmission electron microscopy.</p>
        </caption>
        <graphic xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="microstructures6093.fig.2.jpg" />
      </fig>
      <p>
        <xref ref-type="fig" rid="fig3">Figure 3A</xref>-<xref ref-type="fig" rid="fig3">D</xref> presents the surface SEM images of the four PLSBZST thick-film ceramics and their grain size distributions. All ceramic samples show dense microstructures, clear grain boundaries, closely packed grains, and small pores at multigrain junctions. The inset of each panel shows the grain size distribution histogram obtained using ImageJ software. The grain sizes are mainly distributed between 1 and 3 μm. These fine grain sizes improve the DBS of the ceramics via the relation <inline-formula><tex-math id="M7">$$  E_B\propto G^{-a}  $$</tex-math></inline-formula>, where <italic>E<sub>B</sub></italic> is the DBS, <italic>G</italic> is the average grain size, and <italic>a</italic> is a constant<sup>[<xref ref-type="bibr" rid="B45">45</xref>]</sup>. As shown in <xref ref-type="fig" rid="fig3">Figure 3E</xref>, the cross-sectional SEM image indicates that the thickness of the PLSBZST1 thick-film ceramic is 8.32 ± 0.67 μm, and the thicknesses of the other three samples (PLSBZST2, PLSBZST3, and PLSBZST4) are 7.00 ± 0.20, 7.26 ± 0.07, and 8.59 ± 0.15 m, respectively. The distribution of elements is another important factor affecting the DBS of the dielectric ceramics. An uneven elemental distribution can lead to local dielectric breakdown and eventually failure of the entire ceramic, which is not conducive to improving energy storage performance<sup>[<xref ref-type="bibr" rid="B46">46</xref>]</sup>. <xref ref-type="fig" rid="fig3">Figure 3F</xref> shows the surface morphology and EDS mappings of all elements in the PLSBZST1 thick-film ceramic in the selected area (inside the red box). The elemental maps show that Pb, La, Sr, Ba, Zr, Sn, Ti, and O are evenly distributed throughout the analyzed area, with no obvious elemental aggregation observed, which helps enhance the energy storage performance of these ceramics.</p>
      <fig id="fig3" position="float">
        <label>Figure 3</label>
        <caption>
          <p>(A-D) SEM images of the PLSBZST thick-film ceramics; (E) Cross-sectional SEM image of the PLSBZST1 sample; (F) Surface morphology and SEM-EDS elemental mappings (Pb, La, Sr, Ba, Zr, Sn, Ti, O) of the PLSBZST1 sample; the scale bar for these mappings is shown in (F). SEM: Scanning electron microscopy; PLSBZST: (Pb<sub>0.92-x</sub>La<sub>0.04</sub>Sr<sub>x</sub>Ba<sub>0.02</sub>)(Zr<sub>0.64</sub>Sn<sub>0.35</sub>Ti<sub>0.01</sub>)O<sub>3</sub>; EDS: energy-dispersive X-ray spectrometer.</p>
        </caption>
        <graphic xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="microstructures6093.fig.3.jpg" />
      </fig>
      <p>
        <xref ref-type="fig" rid="fig4">Figure 4A</xref>-<xref ref-type="fig" rid="fig4">D</xref> shows the temperature-dependent relative dielectric constant (<italic>ε<sub>r</sub></italic>) and loss tangent (tanθ) for PLSBZST ceramics at frequencies of 1, 5, 10, and 50 kHz in the temperature range of 30-320 °C. At a constant temperature, the slight decrease in the dielectric constant with increasing measurement frequency is attributed to the reduced ability of dipoles to follow the alternating field at high frequencies<sup>[<xref ref-type="bibr" rid="B43">43</xref>]</sup>. The maximum dielectric constant (<italic>ε<sub>m</sub></italic>) gradually decreases with increasing Sr<sup>2+</sup> content, and the peak temperature (<italic>T<sub>m</sub></italic>) corresponding to <italic>ε<sub>m</sub></italic> also decreases. Due to the influence of the thermodynamic instability of PbSnO<sub>3</sub>, all the samples underwent a stage in which the dielectric constant showed little variation and resulted in a flat, broad peak. This behavior is attributed to the occurrence of a multicell cubic (MCC) phase<sup>[<xref ref-type="bibr" rid="B47">47</xref>]</sup>, which exhibits dielectric characteristics similar to those of the relaxor AFEs. To further examine the relaxor AFE characteristics of PLSBZST thick-film ceramics, the modified Curie-Weiss law was used<sup>[<xref ref-type="bibr" rid="B33">33</xref>]</sup></p>
      <fig id="fig4" position="float">
        <label>Figure 4</label>
        <caption>
          <p>(A-D) Dielectric constant and loss tangent as a function of temperature for PLSBZST thick-film ceramics at 1, 5, 10, and 50 kHz; (E) ln(1/<italic>ε<sub>r</sub></italic>-1/<italic>ε<sub>m</sub></italic>) as a function of ln(<italic>T-T<sub>m</sub></italic>) at 10 kHz. (F) Inverse dielectric constant (1000/<italic>ε<sub>r</sub></italic>) as a function of temperature at 10 kHz; the inset shows <italic>T<sub>m</sub></italic>, <italic>T<sub>B</sub></italic>, and <italic>T<sub>B</sub>-T<sub>m</sub></italic> as a function of the Sr<sup>2+</sup> content. Moreover, the red stars denote <italic>T<sub>m</sub></italic>, while the blue stars denote <italic>T<sub>B</sub></italic>. PLSBZST: (Pb<sub>0.92-x</sub>La<sub>0.04</sub>Sr<sub>x</sub>Ba<sub>0.02</sub>)(Zr<sub>0.64</sub>Sn<sub>0.35</sub>Ti<sub>0.01</sub>)O<sub>3</sub>.</p>
        </caption>
        <graphic xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="microstructures6093.fig.4.jpg" />
      </fig>
      <p><disp-formula> <label>(6)</label> <tex-math id="E6"> $$ \frac{1}{\varepsilon_{r}}-\frac{1}{\varepsilon_{m}}=\frac{\left(T-T_{m}\right)^{\gamma}}{c} $$ </tex-math></disp-formula></p>
      <p>where <italic>T</italic> is the temperature above <italic>T<sub>m</sub></italic>, <italic>ε<sub>r</sub></italic> is the relative dielectric constant at <italic>T</italic>, <italic>ε<sub>m</sub></italic> is the maximum dielectric constant, <italic>C</italic> is the Curie constant, and <italic>γ</italic> is the diffuseness parameter. As shown in <xref ref-type="fig" rid="fig4">Figure 4E</xref>, <italic>γ</italic> increases with increasing x from 1.16 (x = 0.04) to 1.61 (x = 0.10). This indicates that the relaxor AFE characteristics of PLSBZST thick-film ceramics are gradually enhanced under these conditions.</p>
      <p>In <xref ref-type="fig" rid="fig4">Figure 4F</xref>, 1000/<italic>ε<sub>r</sub></italic> as a function of temperature, based on the dielectric constant versus temperature plot, clearly shows the degree of diffuseness. <italic>T<sub>B</sub></italic> is the Burns temperature, defined as the formation of polar nano regions in relaxor ferroelectrics, at which <italic>ε<sub>r</sub></italic> begins to deviate from the Curie-Weiss law. The results show that <italic>T<sub>B</sub>-T<sub>m</sub></italic> and the degree of diffuseness increase with increasing Sr<sup>2+</sup> content. The increase in the diffuse degree and relaxor AFE character is beneficial for refining the P-E hysteresis loop, thus obtaining higher <italic>W<sub>rec</sub></italic> and <italic>η</italic> values<sup>[<xref ref-type="bibr" rid="B31">31</xref>,<xref ref-type="bibr" rid="B32">32</xref>,<xref ref-type="bibr" rid="B48">48</xref>,<xref ref-type="bibr" rid="B49">49</xref>]</sup>.</p>
      <p>
        <xref ref-type="fig" rid="fig5">Figure 5A</xref> and <xref ref-type="fig" rid="fig5">B</xref> shows the P-E and current - electric field (I-E) hysteresis loops for the PLSBZST1-4 thick-film ceramics at room temperature. All PLSBZST ceramic samples show typical AFE hysteresis loops and bimodal current curves. With increasing Sr<sup>2+</sup> content, the P-E hysteresis loop exhibits stronger relaxor AFE characteristics, the I-E current peaks broaden, and the peaks shift towards high electric fields, which indicates that the AFE-FE phase transition electric field increases with x<sup>[<xref ref-type="bibr" rid="B11">11</xref>]</sup>.</p>
      <fig id="fig5" position="float" width="500">
        <label>Figure 5</label>
        <caption>
          <p>(A) P-E and (B) current - electric field (I-E) hysteresis loops obtained at room temperature for PLSBZST thick-film ceramics; (C) E<sub>AFE-FE</sub>, E<sub>FE-AFE</sub>, ΔE, and <italic>P<sub>max</sub></italic>; (D) Weibull distribution of the four samples, with the inset showing the DBS as a function of x; (E) <italic>W<sub>rec</sub></italic> and <italic>η</italic> for four samples; (F) Comparison of the <italic>W<sub>rec</sub></italic> and <italic>η</italic> values of PLSBZST2 with those of recently reported AFE ceramics<sup>[<xref ref-type="bibr" rid="B11">11</xref>,<xref ref-type="bibr" rid="B29">29</xref>,<xref ref-type="bibr" rid="B30">30</xref>,<xref ref-type="bibr" rid="B34">34</xref>,<xref ref-type="bibr" rid="B35">35</xref>,<xref ref-type="bibr" rid="B50">50</xref>-<xref ref-type="bibr" rid="B59">59</xref>]</sup>. P-E: Polarization - electric field; PLSBZST: (Pb<sub>0.92-x</sub>La<sub>0.04</sub>Sr<sub>x</sub>Ba<sub>0.02</sub>)(Zr<sub>0.64</sub>Sn<sub>0.35</sub>Ti<sub>0.01</sub>)O<sub>3</sub>; DBS: dielectric breakdown strength; AFE: antiferroelectric; <italic>P<sub>max</sub></italic>: maximum polarization; <italic>W<sub>rec</sub></italic>: recoverable energy storage density.</p>
        </caption>
        <graphic xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="microstructures6093.fig.5.jpg" />
      </fig>
      <p>The AFE-FE and FE-AFE phase transition electric fields and hysteresis width for the four ceramics (ΔE = E<sub>AFE-FE</sub> - E<sub>FE-AFE</sub>) are shown in <xref ref-type="fig" rid="fig5">Figure 5C</xref>. It can be seen that E<sub>AFE-FE</sub> and E<sub>FE-AFE</sub> increase from 306.08 and <InlineParagraph>260.45 kV/cm</InlineParagraph> for PLSBZST1 to 328.68 kV/cm and 287.99 kV/cm for PLSBZST4, and ΔE decreases from <InlineParagraph>45.63 kV/cm</InlineParagraph> for x = 0.04 to 34.59 kV/cm for x = 0.06, then increases with increasing x (x = 0.08, 0.10). Doping the A sites with elements of smaller ionic radii enhances the stability of the AFE phase and increases the AFE-FE transition field<sup>[<xref ref-type="bibr" rid="B38">38</xref>]</sup>. The increase in E<sub>AFE-FE</sub> and E<sub>FE-AFE</sub> increases the area between the up branch of the P-E loop and the polarization axis, thus increasing the discharged energy density <italic>W<sub>rec</sub></italic>. A decrease in ΔE results in a higher energy storage efficiency <italic>η</italic>. As shown in <xref ref-type="fig" rid="fig5">Figure 5C</xref>, the maximum polarization (<italic>P<sub>max</sub></italic>) gradually decreases with increasing Sr<sup>2+</sup> content. On the one hand, the decrease in <italic>P<sub>max</sub></italic> results from the Pb<sup>2+</sup> ions being replaced by Sr<sup>2+</sup> ions with smaller ionic radii, which leads to the shrinking of the unit cells and hinders the relative displacement and movement space of the ions at the A sites, thereby decreasing the polarization<sup>[<xref ref-type="bibr" rid="B35">35</xref>]</sup>. This also affects the AFE-FE phase transition. With increasing Sr<sup>2+</sup> content, the stability of AFE and the interaction between the two adjacent antiparallel dipoles in the AFE domain increase. Consequently, dipole switching within the AFE unit cells becomes more difficult, fewer dipoles align with the electric field, and the AFE-FE transition shifts to a higher electric field<sup>[<xref ref-type="bibr" rid="B50">50</xref>]</sup>. A similar phenomenon has also been reported for Sr<sup>2+</sup>-doped PbZrO<sub>3</sub>-based AFE ceramics<sup>[<xref ref-type="bibr" rid="B11">11</xref>,<xref ref-type="bibr" rid="B30">30</xref>]</sup>.</p>
      <p>
        <xref ref-type="fig" rid="fig5">Figure 5D</xref> shows the Weibull distribution results used to obtain the DBS. The slopes (βs) of all the Weibull distributions are &gt; 14, indicating that all the specimens have better qualities (e.g., DBS, consistency, narrow distribution of the DBS, <italic>etc.</italic>). The Weibull distribution results show that the PLSBZST2 (x = 0.06) sample demonstrated the highest DBS among the four thick-film ceramics, and it was approximately 7.00 ± 0.20 μm thick. These results indicate that a fine and uniform grain-size distribution, dense microstructure, and small ceramic thickness can effectively improve DBS.</p>
      <p>The <italic>W<sub>rec</sub></italic> and <italic>η</italic> values for the PLSBZST ceramics are shown in <xref ref-type="fig" rid="fig5">Figure 5E</xref> to further investigate the energy storage performance of the PLSBZST ceramics. The PLSBZST2 (x = 0.06) ceramic sample demonstrates the highest <italic>W<sub>rec</sub></italic> and <italic>η</italic> values among all specimens, at 20.09 J/cm<sup>3</sup> and 91.34%, respectively. With increasing Sr<sup>2+</sup> content, <italic>P<sub>max</sub></italic> gradually decreases. However, the <italic>W<sub>rec</sub></italic> values of the PLSBZST3 (x = 0.08) and PLSBZST4 (x = 0.10) ceramic samples are larger than those of PLSBZST1 (x = 0.04) due to the increase in the relaxor AFE characteristics. Finally, as shown in <xref ref-type="fig" rid="fig5">Figure 5F</xref>, the <italic>W<sub>rec</sub></italic> and <italic>η</italic> values for PLSBZST2 are compared with those recently published for AFE ceramics<sup>[<xref ref-type="bibr" rid="B11">11</xref>,<xref ref-type="bibr" rid="B29">29</xref>,<xref ref-type="bibr" rid="B30">30</xref>,<xref ref-type="bibr" rid="B34">34</xref>,<xref ref-type="bibr" rid="B35">35</xref>,<xref ref-type="bibr" rid="B50">50</xref>-<xref ref-type="bibr" rid="B59">59</xref>]</sup>. The enhanced <italic>W<sub>rec</sub></italic> and <italic>η</italic> will be favorable for the larger discharged energy density and higher energy efficiency of the pulse power capacitors.</p>
      <p>The analysis of the P-E hysteresis loops indicated that the PLSBZST2 ceramic sample exhibits the highest <italic>W<sub>rec</sub></italic> among all PLSBZST AFE ceramics. In addition, the stability of <italic>W<sub>rec</sub></italic> with respect to temperature and frequency is an important parameter for evaluating the energy-storage performance of dielectric capacitors<sup>[<xref ref-type="bibr" rid="B60">60</xref>]</sup>. <xref ref-type="fig" rid="fig6">Figure 6A</xref> shows the P-E hysteresis loops of the PLSBZST2 ceramic at 940 kV/cm and 10 Hz over the temperature range of 30-110 °C. The E<sub>AFE-FE</sub>, E<sub>FE-AFE</sub>, ΔE, and <italic>P<sub>max</sub></italic> values as a function of temperature for PLSBZST2 ceramics are shown in <xref ref-type="fig" rid="fig6">Figure 6B</xref>. As temperature increases, the hysteresis loop slightly widens, which can be attributed to the continuous increase in the loss tangent. Moreover, <italic>P<sub>max</sub></italic> decreases almost linearly from 41.13 to 36.86 μC/cm<sup>2</sup> at 940 kV/cm with increasing temperature, which is probably due to the diffuse phase transition from an orthorhombic phase to a MCC phase<sup>[<xref ref-type="bibr" rid="B31">31</xref>]</sup>, whereas ΔE increases from 14.87 to 39.89 kV/cm. The <italic>W<sub>rec</sub></italic> and <italic>η</italic> values as a function of temperature for the PLSBZST2 ceramics are shown in <xref ref-type="fig" rid="fig6">Figure 6C</xref>. With increasing temperature, <italic>W<sub>rec</sub></italic> gradually decreases from 13.39 to 11.65 J/cm<sup>3</sup>, corresponding to a variation of less than 15%. By contrast, <italic>η</italic> is initially constant with increasing temperature and then slightly decreases but remains above 86%. Because temperature does not significantly affect the shape of the P-E hysteresis loop, <italic>W<sub>rec</sub></italic> and <italic>η</italic> values show very small variations with increasing temperature, demonstrating excellent temperature stability. <xref ref-type="fig" rid="fig6">Figure 6D</xref> shows the P-E hysteresis loops for the PLSBZST2 ceramics at 880 kV/cm and room temperature over the frequency range of 0.2-100 Hz. The corresponding E<sub>AFE-FE</sub>, E<sub>FE-AFE</sub>, ΔE, and <italic>P<sub>max</sub></italic> values are shown in <xref ref-type="fig" rid="fig6">Figure 6E</xref> as a function of frequency. With increasing measurement frequency, <italic>P<sub>max</sub></italic> slightly decreases from 40.8 to 39.60 μC/cm<sup>2</sup> at 880 kV/cm, corresponding to a variation of less than 3%, which is due to the small variation in the shape of the P-E hysteresis loop with increasing frequency. E<sub>AFE-FE</sub> and ΔE monotonically increase with increasing frequency, and E<sub>FE-AFE</sub> slightly decreases, resulting in a slowly increasing energy storage density and efficiency for PLSBZST2 [<xref ref-type="fig" rid="fig6">Figure 6F</xref>]. At a low frequency of 0.2 Hz, <italic>W<sub>tot</sub></italic> is the largest among the tested frequencies while <italic>W<sub>rec</sub></italic> is the smallest because of the wide loop, and <italic>η</italic> is only 85.31%. However, at other frequencies from 1 to 100 Hz, <italic>W<sub>rec</sub></italic> increases from 12.44 to 12.86 J/cm<sup>3</sup>, corresponding to a variation of less than 3.4%, while <italic>η</italic> remains above 91%. Overall, the PLSBZST2 ceramics exhibit excellent temperature and frequency stabilities over the measured ranges, indicating their potential for use in pulse power capacitor applications.</p>
      <fig id="fig6" position="float">
        <label>Figure 6</label>
        <caption>
          <p>(A) P-E loops for PLSBZST2 thick-film ceramics at 940 kV/cm from 30 to 110 °C; (B) Corresponding E<sub>AFE-FE</sub>, E<sub>FE-AFE</sub>, ΔE, and <italic>P<sub>max</sub></italic> values obtained at various temperatures; (C) Calculated <italic>W<sub>tot</sub></italic>, <italic>W<sub>rec</sub></italic>, and <italic>η</italic> values obtained at various temperatures; (D) P-E loops for the PLSBZST2 thick-film ceramic at 880 kV/cm from 0.2 to 100 Hz; (E) Corresponding E<sub>AFE-FE</sub>, E<sub>FE-AFE</sub>, ΔE, and <italic>P<sub>max</sub></italic> obtained at various frequencies; (F) Calculated <italic>W<sub>tot</sub></italic>, <italic>W<sub>rec</sub></italic>, and <italic>η</italic> values obtained at various frequencies. P-E: Polarization - electric field; PLSBZST2: (Pb<sub>0.86</sub>La<sub>0.04</sub>Sr<sub>0.06</sub>Ba<sub>0.02</sub>)(Zr<sub>0.64</sub>Sn<sub>0.35</sub>Ti<sub>0.01</sub>)O<sub>3</sub>; <italic>P<sub>max</sub></italic>: maximum polarization; W<italic><sub>tot</sub></italic>: total energy storage density; <italic>W<sub>rec</sub></italic>: recoverable energy storage density.</p>
        </caption>
        <graphic xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="microstructures6093.fig.6.jpg" />
      </fig>
      <p>Moreover, it was observed that the thickness of the ceramic was closely related to the energy storage density. For example, an energy storage density <italic>W<sub>rec</sub></italic> of 20.09 J/cm<sup>3</sup> was obtained at 1,440 kV/cm for a PLSBZST2 ceramic with a thickness of 7.00 ± 0.20 μm. In our previous studies, <italic>W<sub>rec</sub></italic> was 12.9 J/cm<sup>3</sup> at 570 kV/cm for a (PbBaSrLa)(ZrSn)O<sub>3</sub> ceramic with a thickness of 32 μm<sup>[<xref ref-type="bibr" rid="B54">54</xref>]</sup>, 9.84 J/cm<sup>3</sup> at 440 kV/cm for a (PbLa)(ZrSn)O<sub>3</sub> ceramic with a thickness of 50 μm<sup>[<xref ref-type="bibr" rid="B61">61</xref>]</sup>, and 5.72 J/cm<sup>3</sup> at 280 kV/cm for (PbLa)(ZrSnHf)O<sub>3</sub> ceramic with a thickness of 50-70 μm<sup>[<xref ref-type="bibr" rid="B62">62</xref>]</sup>. The energy storage density increases with decreasing thickness in thick-film ceramics. The thickness dependence of the energy storage density reminds us of the general relationship of energy storage density as a function of thickness. Especially whether or not we can figure out a mathematical relation to describe this kind of relation. Furthermore, the thickness dependences of polarization, especially the maximum polarization and DBS, might also be figured out. In fact, the DBS may be related to the thickness via the Gerson-Marshall relation<sup>[<xref ref-type="bibr" rid="B63">63</xref>]</sup>:</p>
      <p><disp-formula> <label>(7)</label> <tex-math id="E7"> $$ E_{D B S}=27.2 t^{-0.39} $$ </tex-math></disp-formula></p>
      <p>where <italic>t</italic> is in cm and <italic>E<sub>DBS</sub></italic> is in kV/cm.</p>
      <p>In general, <italic>E<sub>DBS</sub></italic> can be written as</p>
      <p><disp-formula> <label>(8)</label> <tex-math id="E8"> $$ E_{D B S} \sim t^{s 1} $$ </tex-math></disp-formula></p>
      <p>where <italic>s</italic>1 is a constant, -0.39. Because the polarization is proportional to the electric field, <italic>P</italic> = <italic>ε<sub>r</sub></italic>ε<sub>0</sub><italic>E</italic> for linear ferroelectrics (<italic>ε</italic><sub>0</sub> is the vacuum dielectric constant) and <italic>P~E</italic><sup>2</sup> for nonlinear ferroelectrics (i.e., via the Rayleigh relation and even higher powers<sup>[<xref ref-type="bibr" rid="B64">64</xref>]</sup>), the polarization remains an exponential function:</p>
      <p><disp-formula> <label>(9)</label> <tex-math id="E9"> $$ E_{D B S} \sim t^{s 1} $$ </tex-math></disp-formula></p>
      <p>where <italic>s</italic>2 is also a constant. The recoverable energy storage density is defined as Equation (2) i.e., <inline-formula><tex-math id="M8">$$  W_{rec}=\int EdP $$</tex-math></inline-formula>. Here, because energy storage density is the product of electric field times the polarization, while both the electric field and the polarization have an exponential relationship with the thickness, thereby the energy storage density has an exponential relationship with the thickness, no matter the ferroelectric is a linear ferroelectric (<italic>P vs. E</italic>), or a nonlinear ferroelectric [<italic>P vs. E</italic><sup>2</sup> for Rayleigh relationship, or <italic>P vs. E<sup>n</sup></italic> (<italic>n</italic> &gt; 2)]<sup>[<xref ref-type="bibr" rid="B28">28</xref>]</sup>. Therefore, the recoverable energy storage density exhibits an exponential relationship with the thickness via</p>
      <p><disp-formula> <label>(10)</label> <tex-math id="E10"> $$ W_{r e c} \sim t^{s 0} $$ </tex-math></disp-formula></p>
      <p>where <italic>s</italic>0 is still a constant. Because <italic>W<sub>rec</sub></italic> is the product of the polarization and the electric field, there exists the following relationship among <italic>s</italic>0, <italic>s</italic>1, and <italic>s</italic>2:</p>
      <p><disp-formula> <label>(11)</label> <tex-math id="E11"> $$ s 0=s 1+s 2 $$ </tex-math></disp-formula></p>
      <p>We compared the data obtained with this study with DBS (a)<sup>[<xref ref-type="bibr" rid="B65">65</xref>-<xref ref-type="bibr" rid="B69">69</xref>]</sup>, <italic>P<sub>max</sub></italic> (b)<sup>[<xref ref-type="bibr" rid="B70">70</xref>-<xref ref-type="bibr" rid="B74">74</xref>]</sup>, and <italic>W<sub>rec</sub></italic> (c)<sup>[<xref ref-type="bibr" rid="B75">75</xref>-<xref ref-type="bibr" rid="B79">79</xref>]</sup> data obtained in previous studies as a function of thickness<sup>[<xref ref-type="bibr" rid="B80">80</xref>-<xref ref-type="bibr" rid="B84">84</xref>]</sup> for bulk ceramics, thick film ceramics, and thin films (see <inline-supplementary-material content-type="local-data" mimetype="application/pdf" xlink:href="microstructures6093-SupplementaryMaterials.pdf">Supplementary Table 1</inline-supplementary-material>)<sup>[<xref ref-type="bibr" rid="B11">11</xref>,<xref ref-type="bibr" rid="B31">31</xref>,<xref ref-type="bibr" rid="B33">33</xref>-<xref ref-type="bibr" rid="B35">35</xref>,<xref ref-type="bibr" rid="B41">41</xref>-<xref ref-type="bibr" rid="B43">43</xref>,<xref ref-type="bibr" rid="B55">55</xref>,<xref ref-type="bibr" rid="B56">56</xref>,<xref ref-type="bibr" rid="B85">85</xref>-<xref ref-type="bibr" rid="B93">93</xref>]</sup>. The data were then fitted using Equations (8)-(10), and the results are shown in <xref ref-type="fig" rid="fig7">Figure 7A</xref>-<xref ref-type="fig" rid="fig7">C</xref>. We obtained <italic>s</italic>1, <italic>s</italic>2, and <italic>s</italic>0 values of -0.39 ± 0.03, -0.13 ± 0.03, and -0.43 ± 0.04, respectively. Here, <italic>s</italic>0 is notably less than the sum of <italic>s</italic>1 and <italic>s</italic>2, which likely resulted from the small polarization and electric field used to measure the recoverable energy storage density, because usually the applied electric field used for measuring the recoverable energy storage density is smaller than the DBS, and the polarization obtained at an electric field less than the DBS is smaller than the maximum polarization, and the larger the electric field, the larger the maximum polarization, the DBS and the recoverable energy storage density. Therefore, the absolute value of <italic>s</italic>0 will be less than the absolute sum of <italic>s</italic>1 + <italic>s</italic>2. For example, if less than 10% of each parameter is used, then a 20% error will be generated. Therefore, an <italic>s</italic>0 value of -0.42 will be obtained, which is similar to the actual <italic>s</italic>0 value of -0.43. In addition, it should be noted that the <italic>s</italic>1 value obtained here (-0.39) is the same as that obtained using Equation (7)<sup>[<xref ref-type="bibr" rid="B63">63</xref>]</sup>.</p>
      <fig id="fig7" position="float">
        <label>Figure 7</label>
        <caption>
          <p>Fitted results of the DBS (A)<sup>[<xref ref-type="bibr" rid="B65">65</xref>-<xref ref-type="bibr" rid="B69">69</xref>]</sup>, <italic>P<sub>max</sub></italic> (B)<sup>[<xref ref-type="bibr" rid="B70">70</xref>-<xref ref-type="bibr" rid="B74">74</xref>]</sup> and <italic>W<sub>rec</sub></italic> (C)<sup>[<xref ref-type="bibr" rid="B75">75</xref>-<xref ref-type="bibr" rid="B79">79</xref>]</sup> values as a function of thickness<sup>[<xref ref-type="bibr" rid="B80">80</xref>-<xref ref-type="bibr" rid="B84">84</xref>]</sup> for data extracted from the literature<sup>[<xref ref-type="bibr" rid="B11">11</xref>,<xref ref-type="bibr" rid="B31">31</xref>,<xref ref-type="bibr" rid="B33">33</xref>-<xref ref-type="bibr" rid="B35">35</xref>,<xref ref-type="bibr" rid="B41">41</xref>-<xref ref-type="bibr" rid="B43">43</xref>,<xref ref-type="bibr" rid="B55">55</xref>,<xref ref-type="bibr" rid="B56">56</xref>,<xref ref-type="bibr" rid="B85">85</xref>-<xref ref-type="bibr" rid="B89">89</xref>,<xref ref-type="bibr" rid="B90">90</xref>-<xref ref-type="bibr" rid="B93">93</xref>]</sup>. DBS: Dielectric breakdown strength; <italic>P<sub>max</sub></italic>: maximum polarization; <italic>W<sub>rec</sub></italic>: recoverable energy storage density.</p>
        </caption>
        <graphic xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="microstructures6093.fig.7.jpg" />
      </fig>
      <p>The nominal energy density can be calculated by integrating the electric field with respect to the polarization for the P-E hysteresis loop. Therefore, the actual charging and discharging performance of ceramics can be evaluated using the resistor-inductor-capacitor (R-L-C) circuit<sup>[<xref ref-type="bibr" rid="B30">30</xref>,<xref ref-type="bibr" rid="B94">94</xref>,<xref ref-type="bibr" rid="B95">95</xref>]</sup>. According to the different circuit parameters, the circuit can be divided into an underdamped circuit and an overdamped circuit depending on the load. In an underdamped circuit, the pulse capacitor can release a higher current and thus a higher power density. In an overdamped circuit, the energy stored in the ceramic capacitor can be fully released<sup>[<xref ref-type="bibr" rid="B43">43</xref>]</sup>, which is beneficial for analyzing the actual discharge performance of the ceramics. <xref ref-type="fig" rid="fig8">Figure 8A</xref> shows the discharged current as a function of time for the PLSBZST2 thick-film ceramic obtained under different electric fields in the overdamped circuit. The peak current gradually increases with increasing electric field. The discharged energy density (<italic>W<sub>dis</sub></italic>) may be defined as a function of time for different electric fields during charging, as shown in <xref ref-type="fig" rid="fig8">Figure 8B</xref>. In general, <italic>W<sub>dis</sub></italic> can be calculated via<sup>[<xref ref-type="bibr" rid="B96">96</xref>]</sup></p>
      <fig id="fig8" position="float">
        <label>Figure 8</label>
        <caption>
          <p>Discharge current as a function of time for the PLSBZST2 thick-film ceramic. (A) Overdamped discharge current obtained under various electric fields; (B) Corresponding <italic>W<sub>dis</sub></italic> values obtained under various electric fields; (C) Underdamped discharge current obtained under various electric fields; (D) Corresponding <italic>I<sub>max</sub></italic>, <italic>C<sub>D</sub></italic>, and <italic>P<sub>D</sub></italic> values as a function of the electric field. <italic>I<sub>max</sub></italic>: Peak current; PLSBZST2: (Pb<sub>0.86</sub>La<sub>0.04</sub>Sr<sub>0.06</sub>Ba<sub>0.02</sub>)(Zr<sub>0.64</sub>Sn<sub>0.35</sub>Ti<sub>0.01</sub>)O<sub>3</sub>; <italic>C<sub>D</sub></italic>: discharged current density; <italic>P<sub>D</sub></italic>: discharged power density; <italic>W<sub>dis</sub></italic>: discharged energy density.</p>
        </caption>
        <graphic xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="microstructures6093.fig.8.jpg" />
      </fig>
      <p><disp-formula> <label>(12)</label> <tex-math id="E12"> $$ W_{d i s}=\frac{R \int i(t)^{2} d t}{v} $$ </tex-math></disp-formula></p>
      <p>where <italic>R</italic> is the total resistance in the overdamped circuit (here, <italic>R</italic> = 100 Ω), <italic>i</italic>(<italic>t</italic>) is the discharged current, and <italic>v</italic> is the effective volume of the sample under test. Therefore, <italic>W<sub>dis</sub></italic> increases with increasing electric field. When the electric field approaches 312 kV/cm near the transition field E<sub>AFE-FE</sub>, <italic>W<sub>dis</sub></italic> rapidly increases, and the maximum <italic>W<sub>dis</sub></italic> value of 6.79 J/cm<sup>3</sup> is obtained at 500 kV/cm. The discharge time (<italic>t</italic><sub>0.9</sub>) is defined as the time required to reach 90% of the discharged energy density <italic>W<sub>dis</sub></italic><sup>[<xref ref-type="bibr" rid="B97">97</xref>]</sup>. At an electric field of 500 kV/cm, the PLSBZST2 ceramics can release 90% of <italic>W<sub>dis</sub></italic> in 95 ns, demonstrating rapid discharge. <xref ref-type="fig" rid="fig8">Figure 8C</xref> shows the discharged current as a function of time for the PLSBZST2 ceramic under different electric fields in an underdamped state. Here, the peak current (<italic>I<sub>max</sub></italic>) increases with increasing electric field. The oscillatory pulse current can be evaluated in terms of the discharged current density (<italic>C<sub>D</sub></italic>) and power density (<italic>P<sub>D</sub></italic>)<sup>[<xref ref-type="bibr" rid="B98">98</xref>]</sup>:</p>
      <p><disp-formula> <label>(13)</label> <tex-math id="E13"> $$ C_{D}=\frac{I_{ {max }}}{S} $$ </tex-math></disp-formula></p>
      <p><disp-formula> <label>(14)</label> <tex-math id="E14"> $$ P_{D}=\frac{E I_{{max }} }{2 S}  $$ </tex-math></disp-formula></p>
      <p>where <italic>I<sub>max</sub></italic> is the peak value of the first pulse current, E is the charging electric field, and <italic>S</italic> is the electrode area of the sample. <italic>I<sub>max</sub></italic>, <italic>C<sub>D</sub></italic>, and <italic>P<sub>D</sub></italic> are shown as functions of the electric field in <xref ref-type="fig" rid="fig8">Figure 8D</xref>. Here, <italic>I<sub>max</sub></italic>, <italic>C<sub>D</sub></italic>, and <italic>P<sub>D</sub></italic> monotonically increase with increasing electric field, and a pronounced increase occurs near the AFE-FE transition field. The maximum <italic>C<sub>D</sub></italic> and <italic>P<sub>D</sub></italic> values of 687.73 A/cm<sup>2</sup> and 128.95 MW/cm<sup>3</sup>, respectively, are obtained under an electric field of 375 kV/cm. These results demonstrate that the PLSBZST2 ceramic exhibits a high discharged energy density, high discharged current, high power density, and short discharge time, indicating its potential for application in pulse-power devices.</p>
    </sec>
    <sec id="sec4">
      <title>CONCLUSIONS</title>
      <p>In this study, (Pb<sub>0.92-x</sub>La<sub>0.04</sub>Sr<sub>x</sub>Ba<sub>0.02</sub>)(Zr<sub>0.64</sub>Sn<sub>0.35</sub>Ti<sub>0.01</sub>)O<sub>3</sub> (PLSBZST; x = 0.04, 0.06, 0.08 and 0.10) freestanding thick-film ceramics were successfully fabricated using the tape-casting process. The results show that the forward AFE-FE switching field and relaxor degree increase with increasing Sr<sup>2+</sup> content, while a fine grain size and dense microstructure are beneficial for improving the DBS. In particular, the PLSBZST2 thick-film ceramic demonstrated a maximum <italic>W<sub>rec</sub></italic> of 20.09 J/cm<sup>3</sup> with an <italic>η</italic> of 91.34% at 1,440 kV/cm, together with excellent frequency and temperature stabilities and an excellent discharging performance. In addition, under a load of 100 Ω, the PLSBZST2 ceramic exhibited a maximum <italic>W<sub>dis</sub></italic> value of 6.79 J/cm<sup>3</sup> at 500 kV/cm and released 90% of this <italic>W<sub>dis</sub></italic> value within 95 ns. Moreover, maximum <italic>C<sub>D</sub></italic> and <italic>P<sub>D</sub></italic> values of 687.73 A/cm<sup>2</sup> and 128.95 MW/cm<sup>3</sup> were obtained. These findings indicate the potential of PLSBZST thick-film ceramics for use in pulse-power devices. Moreover, reciprocal exponential relationships of the maximum polarization, DBS, and <italic>W<sub>rec</sub></italic> as a function of the sample thickness were obtained. The <italic>s</italic>2, <italic>s</italic>1, and <italic>s</italic>0 exponents associated with these relationships were -0.13 ± 0.03, -0.39 ± 0.03, and -0.43 ± 0.04, respectively. Here, the value of exponent <italic>s</italic>1 is the same as that obtained using the Gerson-Marshall equation, and <italic>s</italic>0 is almost equal to (<italic>s</italic>1 + <italic>s</italic>2)  80%, which results from using 10% less than the maximum polarization and a lower electric field than that used for the DBS due to the lower electric field that was employed during measurement. The thickness dependence of the recoverable energy storage density directly indicates that the reduction on the thickness of the ceramic layer will be one of the important approaches to enhance the energy storage density for the pulse power capacitors.</p>
    </sec>
  </body>
  <back>
    <sec>
      <title>DECLARATIONS</title>
      <sec>
        <title>Authors’ contributions</title>
        <p>Conception and design: Lu, S. G.; Wang, S.; Yan, X.</p>
        <p>Experiments, data collection and analysis, data curation: Yan, X.; Yu, C.; Li, Y.</p>
        <p>Writing of the original draft: Yan, X.; Wang, S.</p>
        <p>Writing - review and editing: Lu, S. G.; Gao, X.; Wang, S.; Yao, Y.; Tao, T.; Liang, B.; Gong, W.; Niu, X.; Jian, X.</p>
        <p>Supervision, project administration and funding acquisition: Lu, S. G.; Gao, X.; Jian, X.</p>
      </sec>
      <sec>
        <title>Availability of data and materials</title>
        <p>The data supporting the findings of this study are available within this Article and its Supplementary Materials. Further data are available from the corresponding authors upon request.</p>
      </sec>
      <sec>
        <title>AI and AI-assisted tools statement</title>
        <p>Not applicable.</p>
      </sec>
      <sec>
        <title>Financial support and sponsorship</title>
        <p>This work was supported by the Natural Science Foundation of China (Grant Nos. 52272105, 52202130, 52402161), the NSFC-Guangdong Joint Fund (Grant No. U1501246), the State Key Laboratory of Precision Electronic Manufacturing Technology and Equipment-opening fund (JMDZ202305), the Dongguan City Frontier Research Project (2019622101006), the Advanced Energy Science and Technology Guangdong Provincial Laboratory Foshan Branch-Foshan Xianhu Laboratory Open Fund-Key Project (Grant No. XHT2020-011), the Open Projects of the Guangdong Provincial Key Laboratory of Electronic Functional Materials and Devices, Huizhou University [grant numbers EFMD2022004Z and EFMD2024007Z], the Open Project of the Guangdong Provincial Key Laboratory of Energy Conversion Materials and Technology, Guangdong Technion-Israel Institute of Technology [MATEC2024KF003], and the Taishan Industrial Experts Program [No. tscx202507141].</p>
      </sec>
      <sec>
        <title>Conflicts of interest</title>
        <p>Gao, X. is affiliated with Shandong Industrial Ceramics Research and Design Institute Co., Ltd. The other authors declared that there are no conflicts of interest.</p>
      </sec>
      <sec>
        <title>Ethical approval and consent to participate</title>
        <p>Not applicable.</p>
      </sec>
      <sec>
        <title>Consent for publication</title>
        <p>Not applicable.</p>
      </sec>
      <sec>
        <title>Copyright</title>
        <p>© The Author(s) 2026.</p>
      </sec>
      <sec sec-type="supplementary-material">
        <title>Supplementary Materials</title>
        <supplementary-material content-type="local-data">
          <media xlink:href="microstructures6093-SupplementaryMaterials.pdf" mimetype="application/pdf">
            <caption>
              <p>Supplementary Materials</p>
            </caption>
          </media>
        </supplementary-material>
      </sec>
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