Stacking pattern effect on the energy storage performance of PLZT-based relaxor- ferroelectric/antiferroelectric multilayer thin film capacitors prepared by sol-gel methods

Stacking pattern effect on the energy storage performance of PLZT-based relaxor- ferroelectric/antiferroelectric multilayer thin film capacitors prepared by sol-gel methods | Research Square window.SnipcartSettings = { analytics: { enabled: false } }; (function() { var accessVector = localStorage.getItem('access_vector') || ''; window.dataLayer = window.dataLayer || []; if (accessVector) { window.dataLayer.push({ user: { profile: { profileInfo: { snid: accessVector } } } }); } })(); (function(w,d,s,l,i){w[l]=w[l]||[];w[l].push({'gtm.start':new Date().getTime(),event:'gtm.js'});var f=d.getElementsByTagName(s)[0],j=d.createElement(s),dl=l!='dataLayer'?'&l='+l:'';j.async=true;j.src='https://www.googletagmanager.com/gtm.js?id='+i+dl;f.parentNode.insertBefore(j,f);})(window,document,'script','dataLayer','GTM-K279D39R'); Browse Preprints In Review Journals COVID-19 Preprints AJE Video Bytes Research Tools Research Promotion AJE Professional Editing AJE Rubriq About Preprint Platform In Review Editorial Policies Our Team Advisory Board Help Center Sign In Submit a Preprint Cite Share Download PDF Research Article Stacking pattern effect on the energy storage performance of PLZT-based relaxor- ferroelectric/antiferroelectric multilayer thin film capacitors prepared by sol-gel methods Chang Gao, Lijuan Huang, Qi Liu, Shize Wu, Zedong Xu, Chunlin Zhao, and 3 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-7912657/v1 This work is licensed under a CC BY 4.0 License Status: Published Journal Publication published 22 Jan, 2026 Read the published version in Journal of Materials Science: Materials in Electronics → Version 1 posted You are reading this latest preprint version Abstract Lead-based multilayer thin film capacitors with excellent energy storage performances have great application potential. However, the effect of stacking patterns on the dielectric behaviors has not been well investigated, especially for the multilayer thin films prepared by chemical solution methods. Here, the relaxor ferroelectric (RFE) (Pb 0.92 La 0.08 )(Zr 0.65 Ti 0.35 )O 3 and antiferroelectric (AFE) (Pb 0.98 La 0.02 )(Zr 0.95 Ti 0.05 )O 3 were chosen to construct diverse multilayer thin film capacitors with different RFE/AFE stacking patterns. Based on their crystal structure, dielectric features, and energy storage behaviors, the effect of stacking orders and AFE phase thicknesses on the capacitor performances were discussed from the perspectives of the positive and negative interface contribution. A superior recoverable energy density of 26.28 J cm − 3 was achieved at a breakdown strength of 3.19 MV cm − 1 , accompanied with thermal stability up to 170°C, frequency stability up to 2 kHz, and fatigue endurance after 10 6 charging-discharging cycles. The experimental results and related discussion will support the research and the industrialization of multilayer thin film capacitors. Multilayer thin film antiferroelectrics relaxor ferroelectrics energy storage PLZT Figures Figure 1 Figure 2 Figure 3 Figure 4 Figure 5 Figure 6 1. Introduction Dielectric thin films have great potential in micro-scale energy storage devices due to their ultrahigh power density, fast charge/discharge speed, and long lifespan [ 1 ]. To improve recoverable energy storage density ( W rec ) and the efficiency ( η ), it is imperative to increase both the maximum polarization ( P max ) and the electric breakdown strength ( E b ), and reduce the remanent polarization ( P r ). Many strategies have been proposed, such as doping modifications, strain engineering, thickness optimization, and constructing of multilayers [ 2 ]. Various multilayer thin film configurations consisting of ferroelectric (FE), relaxor ferroelectric (RFE), and antiferroelectric (AFE) thin films have been designed [ 1 , 3 – 5 ]. It has been reported that the (AFE/RFE) n -type (PbZrO 3 /Pb 0.9 La 0.1 Zr 0.52 Ti 0.48 O 3 ) 8 multilayers prepared by laser pulsed deposition (PLD) exhibited an enhanced energy storage density with high efficiency ( W rec of 128.4 J cm − 3 and η of 81.2% at the BDS of 4.2 MV cm − 1 ) due to the polarization coupling at the interfaces via epitaxial strains [ 6 ]. However, such physical vapor deposition methods like PLD are not convenient for large-scale industrial production. Chemical methods like the sol-gel/spin coating method can easily prepare multilayer thin films with simple equipment at low cost [ 7 , 8 ]. Unlike the epitaxial multilayers prepared by PLD, the chemically prepared polycrystalline multilayers may benefit less from the interface strain coupling. Still, the interfaces contribute to the improvement in energy storage density. Such positive interface effect is attributed to the blocking of the growth and propagation of electrical trees [ 9 ]. However, the negative interface effect also exists where the lattice mismatch may induce a large number of defects at the interface regions, impairing BDS. Considering that both the positive and negative interface effects are closely related to the multilayer period and the thickness of individual layer, it is important to investigate their effects on the energy storage performances of dielectric multilayer thin films. Lanthanum doped lead zirconate titanate (PLZT) is one of the most studied dielectric materials [ 10 ]. According to its phase diagram, PLZT exhibits the FE feature at the titanate-rich region and the AFE feature at the zirconate-rich region [ 11 ]; whereas the dope of lanthanum is an effective approach to breaking the long-term ordering of electrical dipoles, stabilizing the AFE phase to the low-zirconate region or inducing the RFE phase in the FE region [ 12 – 14 ]. The PLZT thin films with the RFE phase have been evidenced as excellent energy storage media with ultrahigh energy storage efficiencies due to its slim hysteresis loops ( P - E loops) and low P r [ 15 ]. However, the relatively low P max of RFE PLZT limits its maximum energy storage density. On the other hand, the AFE PLZT thin films show double P - E loops and almost zero P r value [ 16 ], making it favourable for energy storage applications, too. It has been reported that the PLZT multilayer thin films consisting of both AFE and RFE phases show better energy storage performances [ 17 ], where the stacking pattern is a key factor that affects the interface density. However, since the thickness of individual layer prepared by the sol-gel/spin coating method can hardly be adjusted, the thickness effect has rarely been investigated, though the ratio of the AFE phase to the entire multilayer thin film could significantly modify the shape of the P - E loops. Herein, the PLZT multilayer thin films with different RFE/AFE stacking patterns were prepared by the sol-gel/spin-coating method. The thickness of AFE layers were adjusted by changing the stacking patterns, and the thickness effect on the energy storage performances of the multiplayer thin film was investigated. The BDS was enhanced due to the interface effect. As the result, the energy storage density of 26.28 J cm − 3 was achieved in the designed PLZT multilayer thin film. 2. Experimental procedure The RFE-type (Pb 0.92 La 0.08 )(Zr 0.65 Ti 0.35 )O 3 (denoted as R) and AFE-type (Pb 0.98 La 0.02 )(Zr 0.95 Ti 0.05 )O 3 (denoted as A) were chosen as the RFE and AFE phases in the PLZT multilayer thin films, respectively. The PLZT multilayer thin films with various AFE/RFE stacking patterns were prepared on the Pt/Ti/SiO 2 /Si substrates by the sol-gel/spin-coating method. Initially, the raw materials were precisely weighed to match the atomic ratio requirements. To compensate for the loss of Pb during the heat treatment, an excess of 10% Pb was used in the precursor solution. Lead acetate trihydrate (PbC 4 H 6 O 4 ·3H 2 O, 99.99%, Aladdin) and lanthanum nitrate hexahydrate (LaN 3 O 9 ·6H 2 O, 99%, Aladdin) were stirred in 2-Methoxyethanol (C 3 H 8 O 2 , AR, Aladdin) for 2 h at 70°C, forming Solution A. Simultaneously, zirconium propoxide (C 12 H 28 O 4 Zr, 70 wt.%, Aladdin) and titanium butoxide (C 16 H 36 O 4 Ti, ≥ 99.0%, Aladdin) were stirred in 2-Methoxyethanol for 1 h at room temperature. An appropriate amount of acetylacetone (C 5 H 8 O 2 , 99%, Aladdin) and formamide (CH 3 NO, 99%, Aladdin) were added as chelating agents to stabilize the solution, forming Solution B. Then, Solution B was mixed with Solution A, and the pH was adjusted by adding a certain amount of glacial acetic acid (CH 3 COOH, AR, Sinopharm Chemical Reagent Co.), followed by continuous stirring at 70°C for 2 h to obtain precursor sols. The precursor solution was aged for 48 h. Then, each layer was spin-coated on the substrate at 4000 rpm for 30 s. The as-grown films were heated on a hot plate at 100 ℃ for 2 min and pyrolyzed in a tube furnace at 450 ℃ for 5 min. Such procedures were repeated several times using different precursors to construct desired stacking patterns. The stacking orders of multilayers were R/A/R/A/R/A, R/A/R/A, R/A/A/R/A/A, and R/A/A/A/R/A/A/A, denoted as (RA) 3 , (RA) 2 , (RAA) 2 , and (RAAA) 2 , respectively. For comparison, the pure RFE (6R layers, R 6 ) and AFE thin films (6A layers, A 6 ) were also prepared. The schematics of all the above multilayer thin film structures are shown in Fig. 1 . Finally, the thin films were crystallized using a rapid thermal annealing furnace at 700 ℃ for 30 min with heating rate was 15 ℃/s. The crystal structure of the multilayer thin films was determined using X-ray diffraction (XRD, Ultima III, Rigaku) with a Cu K α radiation. A pseudocubic (PC) index was used when discussing crystal structures in this text. The local crystal structure and domain distribution of the (RAA) 2 multilayer thin film was measured using transmission electron microscopy (TEM, Talos F200I, FEI) with a working voltage of 200 kV. The TEM sample was prepared by the focusing ion beam (FIB, Helios G4 CX, FEI). The thickness of thin films was measured using field-emission scanning electron microscopy (FESEM, Supra 55, Carl Zeiss). The surface morphology was observed using atomic force microscopy (AFM, MFP-3D, Asylum Research). The Raman spectra were measured using the Raman spectrometer (DXR-2Xi, Thermo Fisher Scientific) with a laser excitation at 532 nm wavelength. The polarization ( P–E ) and current ( I–E ) hysteresis loops of thin films were measured using a ferroelectric analyzer (AIX ACT, TF2000) at 1 kHz, from which the W rec and η were calculated by the following equations: $$\:{W}_{\text{t}\text{o}\text{l}}=\:{\int\:}_{0}^{{P}_{max}}EdP={W}_{rec}+\:{W}_{\text{l}\text{o}\text{s}\text{s}}$$ 1 $$\:{W}_{rec}=\:{\int\:}_{{P}_{r}}^{{P}_{max}}EdP$$ 2 $$\:\eta\:=\:\frac{{W}_{rec}}{{W}_{tol}}\:\times\:100\%$$ 3 where P max is the maximum polarization, P r is the remanent polarization, E is the applied electric field, P is the polarization, and W loss is the energy loss density. For the performance stability measurements, P–E loops of the (RA) 2 multilayer thin film were tested up to 10 6 cycles with pulses of 0.5 kHz − 2 kHz using 1.25 MV cm − 1 as the switching field. For the thermostability, the P–E loops of the same sample were measured with temperature increasing to 170 ℃. 3. Results 3.1. The morphology and structure of PLZT multilayer thin films The AFM images in Figure S1 exhibit smooth surfaces for all the samples with the roughness less than 3.5 nm. The cross-sectional SEM images in Figure S2 suggest the thickness of different samples is between 247 nm (4 layers) and 497 nm (8 layers), corresponding to a thickness of 65 nm for each individual layer. The XRD patterns in Fig. 2 a and 2 c suggest that all the PLZT multilayer thin films exhibit the pure perovskite phase. In order to further analyse the effect of different stacking orders on the structure, a magnified view around the (002) peaks are presented in Fig. 2 b, where significant shifts are observed. The (002) peak of A 6 is located at 2θ = 43.87 ° (corresponding to a lattice parameter c of 0.4124 nm), while that of R 6 is located at 2θ = 44.34 ° (c = 0.4082 nm). For multilayers, the (002) peak of (RAA) 2 film is located at 2θ = 43.90 ° (c = 0.4122 nm), and that of (RA) 3 film is located at 2θ = 43.97 ° (c = 0.4116 nm). Such shift is attributed to the lattice mismatch between the R and A phases (1.02%). In Fig. 2 d, the multilayer films with the same stacking order but different AFE layer thicknesses exhibit almost the same (002) peak location ((RA) 2 : 43.92 °, (RAA) 2 : 43.90 °, (RAAA) 2 : 43.89 °), which corresponds to a 0.05% fluctuation in the lattice constant. However, the decrease of the full width half maximum (FWHM) with the decreasing thickness suggests that the internal stress inside the multilayer thin films is increased due to the lattice mismatch. Figure 2 e shows the cross-sectional TEM image of the (RAA) 2 multilayer thin film, where the dense multilayer structure with the distinguishable R/A interfaces is observed. Specifically, in the R layer (Position ① in Fig. 2 e), nanodomains with a size of 10 nm are observed, evidencing the existence of polar nanoregions (PNRs) for RFEs. Figure 2 f and 2 g show the high-resolution TEM (HRTEM) images and the corresponding selected area electron diffraction (SAED) patterns of the R layer, respectively, where only the lattice reflections are observed. Meanwhile, the SAED pattern ( Fig. 2 i) of the A layer (Position ② in Fig. 2 e) exhibits the (011) superlattice reflections, which represents a periodic antiparallel arrangement of Pb 2+ ions and reveals the AFE nature of the A layer[ 18 , 19 ]. The Raman spectra of the multilayer thin films with different stacking orders are plotted in Figure S3a in the Supplementary Material. The Raman spectra exhibit characteristic peaks at 129 cm⁻¹, 233 cm -1 , 341 cm⁻¹, and 525 cm⁻¹, corresponding to Pb-(ZrO₃) lattice mode, Zr-O bending mode, ZrO₃ twisting mode, and Zr-O/Ti-O bending modes, respectively[ 20 ]. Among them, the Pb-(ZrO 3 ) lattice mode is related to the AFE orthorhombic phase, whose disappearance in the samples other than the A 6 thin film indicates the suppression of AFE phase by introducing the RFE layer [ 16 , 21 ]. Figure S3b shows the Raman spectra of multilayer thin films with different thicknesses of the AFE layers. With the increase of thickness, the Raman peaks at both 233 cm -1 and 525 cm -1 shift slightly towards the higher wave number direction ( i.e. , the peak position of the pure R 6 phase), which associates with the enhanced octahedral torsion and structural distortion, indicating that the structure of multilayer thin films progressively transforms into a RFE-like mode [ 22 ]. 3.2. The effect of the stacking order on the energy storage performance The P–E and I–E curves of the thin films with different stacking orders are measured at 0.85 MV cm − 1 and 1 kHz, as shown in Fig. 3 . A 6 exhibits a double P–E loop with four sharp current-switching peaks in the I–E curve, evidencing the reversible AFE-FE phase transition. For comparison, R 6 shows a typical RFE-like slender P–E loop. Interestingly, (RA) 3 and (RAA) 2 multilayer thin films exhibit different dielectric features. The AFE-like switching behavior is only observed in the (RA) 3 multilayer thin film, evidenced by the corresponding I–E curve, whereas the (RAA) 2 one exhibits a RFE-type P–E loop. Such difference in dielectric features is attributed to the different AFE/RFE stacking orders that may affect the interface strain condition and the thin film crystallinity inside each layer [ 23 ]. The unipolar P–E loops of the multilayer thin films at their BDS are shown in Fig. 4 a- 4 d. Figure 4 e shows that P max of the (RAA) 2 and (RA) 3 multilayer thin films are 57.12 µC cm − 2 at 2.72 MV cm − 1 and 44.8 µC cm − 2 at 2.54 MV cm − 1 , respectively, which are larger than that of the pure A 6 thin films. The introduction of the RFE layers leads to an enhanced P max value in the multilayer thin film [ 22 ]. A near-zero P r value is detected for A 6 and R 6 , whereas the multilayer thin films exhibit nonnegligible P r . It is due to the inhibition of domain switching as the defect density is increased by inducing the AFE/RFE interfaces. Since the (RA) 3 multilayer thin film has more R/A interfaces than the (RAA) 2 one, the ΔP of (RA) 3 is smaller than that of (RAA) 2 . Figure 4 f shows that the W rec of A 6 , R 6 , (RA) 3 , and (RAA) 2 samples are 18.8 J cm − 3 ,16.2 J cm − 3 ,11.96 J cm − 3 and 18.74 J cm − 3 , respectively, and their η are 48%, 48.66%, 19.3%, 41.09%, respectively. The fitting BDS from the Weibull distributions for A 6 , R 6 , (RA) 3 and (RAA) 2 thin films are 1.93, 1.803, 2.54, and 2.72 MV cm − 1 , respectively, as shown in Fig. 4 g, in consistence with the results in Fig. 4 a- 4 d. In sum, the multilayer thin films with three R/A interfaces show better energy storage performances than those with five R/A interfaces. 3.3. The effect of the thickness on energy storage performance Next, the energy storage properties of (RA) 2 , (RAA) 2 , and (RAAA) 2 multilayer thin films were compared. Note that these three samples have the same interface number but different AFE layer thicknesses. As shown in Fig. 5 a -Figure 5c , (RA) 2 exhibits thinnest P – E loops with four obvious peaks in the I – E loops, suggesting a relaxor AFE (RAFE) feature. Such results indicate that the (RA) 3 multilayer films might have also belonged to the RAFE phase because they have similar stacking orders. However, the negative interface effect induces defects that “broaden” the P – E loops (Fig. 3 c). With the increasing thickness of AFE layers, the multilayer thin films trend to exhibit the RFE feature in (RAA) 2 and the FE one in (RAAA) 2 . As the result, the P r value is gradually increased. Figure 5 d illustrates the unipolar P – E loops of films with different AFE layer thicknesses at E b . With the increase of AFE layer thickness, E b decreases. Such phenomena are attributed to the thicker thickness that weaken the positive interfacial effect[ 24 ]. Therefore, the good energy storage performance in the (RFE/AFE) 2 -type multilayers might probably be attributed to the positive interface effect. As shown in Fig. 5 e, with the increase of AFE layer thickness, the P max changes little, ΔP first increases then decreases. The W rec of (RA) 2 , (RAA) 2 and (RAAA) 2 multilayer thin films is 26.28 J cm − 3 , 18.74 J cm − 3 and 17.17 J cm − 3 , respectively, the corresponding η is 49.78%, 41.09% and 58.86%, respectively, as shown in Fig. 5 f. Compared to the A 6 AFE thin films, the W rec of (RA) 2 is improves by 7.48 J cm − 3 . For dielectric energy storage materials, reliability and stability is the key factors to evaluate the performance. Figure 6 shows the energy storage reliability of (RA) 2 multilayer thin films at various frequencies, temperature, and cycles, respectively. The (RA) 2 multilayer thin films have excellent frequency stability in the range of 0.5 kHz to 2 kHz, good temperature stability up to 170℃, and cycling reliability up to 10 6 cycles, ensuring the (RA) 2 multilayer thin film a promising candidate for energy storage capacitors. 4. Discussion Publications have reported that the RFE PLZT (8/65/35) and the AFE PLZT(2/95/5) exhibit a rhombohedral structure and an orthorhombic structure, respectively[ 25 ]. The XRD patterns in Fig. 2 confirm such difference in structure. More importantly, all the multilayer thin films with various stacking patterns (either different stacking orders or different AFE layer thicknesses) exhibit a similar lattice constant value with the AFE A 6 sample (check Fig. 2 b and 2 d), indicating the AFE orthorhombic phase (AFE O ) is dominating in all these multilayer thin films through they have several RFE layers inside. However, the P – E curves and corresponding I – E curves in Fig. 3 and Fig. 5 indicate diverse dielectric features in the multilayer thin films with different stacking patterns. In detail, (RA) 3 , (RA) 2 , (RAA) 2 , and (RAAA) 2 show the AFE, RAFE, RFE, and FE phases, respectively. Among them, the (RA) 3 multilayer film might have also belonged to the RAFE phase because it has a similar stacking order with (RA) 2 . However, the negative interface effect induces defects that “broaden” the P – E loops (Fig. 3 c). Additionally, please note that the superlattice diffraction pattern in Fig. 2 i evidences the existence of AFE phase in the (RAA) 2 multilayer thin film. The contradictory results between the SAED pattern and dielectric tests indicate the significant difference between the apparent and the local dielectric features in the (RAA) 2 multilayer thin film. Besides, it is interesting to find a FE feature in the multilayer thin film with the thickest AFE layers, where the reason needs further investigation. According to the above discussion, although different multilayer thin films exhibit similar apparent crystal structure, their dielectric features are diverse, leading to different energy storage performances. Amongst them, (RA) 2 shows the best energy storage performance with W rec of 26.28 J cm -3 and η of 49.78%. The energy storage properties of multilayer thin films depend on P max , P r , E A , E F , and E b of samples, which is determined by the stacking patterns based on the interlayer coupling effect [ 26 , 27 ]. By modifying the stacking patterns, it is possible to construct various heterogeneous interface conditions in the multilayer thin films that may thus influence the energy storage performance in a positive or negative way[ 28 – 30 ]. First, the interfacial blocking effect serves as a critical barrier against the growth and spread of electrical trees [ 6 , 31 ]. Thus, a larger interface density could effectively enhance E b (check Fig. 4 a- 4 d) and make positive contribution to the energy storage performance. However, the lattice mismatch between R and A phases induces significant interfacial stress [ 32 ]. Thus, the larger interface density would result in more defects at the interfaces region that promotes the generation of leakage currents (check the P – E loops in Fig. 3 ), negatively affecting energy storage efficiency. As the result, it is a trade-off to design modest interface density to improve energy storage performance. As illustrated in Fig. 1 , (RA) 3 contains two additional R/A interfaces compared to (RAA) 2 , leading to an increased energy loss density but the similar E b , and thus poorer energy storage performance (check Fig. 4 ) . Note that the interface stress effect is correlated to the fabrication methods. Some physical vapor deposition methods like PLD may induce a large amount of epitaxial stress (although some literature reported that such stress may enhance P max )[ 33 ], whereas the chemical solution method like sol-gel/spin-coating could reduce the interfacial stress effect by the proper annealing process[ 34 , 35 ]. Second, the thickness effect may also influence energy storage performance. Generally, reducing the thickness may impair the crystallinity of layers and increase the defects inside, increasing the energy loss density. However, such negative effects have a critical thickness (usually several tens of nanometers[ 36 , 37 ]) and are affected by the interfacial condition. In our cases, increasing the thickness of AFE layer (without changing the stacking orders) indeed decreases the energy loss density and improves the energy storage efficiency. However, the dielectric features of multilayer thin films have also changed, which leads to a decrease in energy storage density with increasing AFE layer thickness (check Fig. 5 d). The AFE phase thickness is controlled by stacking different numbers of AFE layers (65 nm per layer). Thus, the fact that the dielectric features would change from RAFE to FE phases indicates that the A/A interface condition also affects the dielectric behaviors. The lattice mismatch at the A/A interfaces caused by multiple spin-coating deposition sequences may also induce defects that could generate leakage current and might inhibit AFE-FE phase transition in a worse situation[ 38 ]. A layer-by-layer annealing approach may weaken the effect of such A/A lattice mismatch, but it is much more time-consuming and energy-costing. As shown in Fig. 6 d and Table 1 , the (RA) 2 multilayer film has superior E b and thus W rec , in comparison with other PZ-based FE/AFE multilayer thin films. Table 1 summarizes the energy storage property densities of (RA) 2 multilayers and other AFE, RFE, and FE/AFE multilayer films. Ref. W rec (J cm -3 ) η (%) E (MV cm -1 ) Materials Types Preparation technique This work 26.28 9.59 49.28 62.25 3.19 1.25 PLZT PLZT AFE/RFE AFE/RFE Sol-Gel Sol-Gel Sheng Tong et al[ 39 ] 22 77 1.6 PLZT/LNO RFE Sol-Gel Ngo Duc Quan et al[ 40 ] 8.1 56.2 0.35 PLZT/BNKT RFE Sol-Gel Jie Zhang et al[ 41 ] 21.11 63.3 1.373 PZT/PZO FE/AFE Sol-Gel Fei Yang et al[ 37 ] 32.4 66.9 2.745 PZT/PZO FE/AFE Sol-Gel Fei Yang et al[ 42 ] 10.0 84.8 1.975 PZT/PZO/LNO FE/AFE Sol-Gel Chao Yin et al[ 43 ] 16.6 50.4 0.7841 PZO/LNO AFE Sol-Gel M. M. Zheng et al[ 44 ] 8.7 93.1 1.5 PZO AFE Sol-Gel Nguyen CTQ et al[ 45 ] 12.74 88.44 1 PZT/PLZT RFE/AFE PLD Pan et al[ 46 ] 20 74.1 1.2 PLZT AFE CSD Zhong Qiang Hu et al[ 15 ] 30 78 2.59 PLZT RFE CSD X. G. Fang et al[ 47 ] 15.3 56 1 PLZT/LNO AFE CSD Balaraman et al[ 38 ] 21 94 1.285 PLZT AFE/RFE CSD Yi Zhuo Li et al[ 48 ] 10.8 60 0.6 Au/PLZT AFE CSD Yinuo Duan et al[ 49 ] 15.26 66.03 1.401 PZO/STO RFE/AFE CSD Yin Chao et al[ 50 ] 28.1 80.1 1.3481 PZO/AO AFE CSD 4. Conclusion (RFE/AFE) n PLZT multilayer thin films with various stacking patterns were prepared by the sol-gel/spin-coating method. The effect of stacking orders and AFE layer thicknesses on the energy storage performances were systematically discussed based on the experimental results. An energy storage density of 26.28 J cm − 1 was obtained in (RA) 2 multilayer thin films, which was attributed to the increase in breakdown strength due to the positive interfacial effect. Moreover, the (RA) 2 multilayer thin film exhibits good thermal stability up to 170°C, good frequency stability up to 2kHz, and excellent fatigue endurance after 10 6 charging-discharging cycles. The study provides useful guidelines for designing PLZT-based multilayer thin film capacitors for pulsed power applications. Declarations Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper. Competing Interests Declaration of Competing InterestThe authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper. Author Contribution Chang Gao: Investigation, Data curation. Lijuan Huang: Methodology, Conceptualization. Chunlin Zhao: Resources, Supervision. Xiao Wu: Resources, Supervision. Tengfei Lin: Resources, Supervision. Cong Lin: Resources, Supervision. Min Gao: Conceptualization, Writing – review & editing, Funding acquisition. Acknowledgement The authors appreciate the support of the National Natural Science Foundation of China (52102126, 52072075, and 12104093), the Natural Science Foundation of Fujian Province (2022J01087, 2022J015552, 2021J05122 and 2021J05123), and the Open Project of Tianjin Key Laboratory of Optoelectronic Detection Technology and System (2024LODTS101). Data Availability The data that support the findings of this study are available from the corresponding author upon reasonable request. References H. Palneedi, M. Peddigari et al., High-performance dielectric ceramic films for energy storage capacitors: progress and outlook. Adv. Funct. Mater. (2018). 28.(42). .http://doi.org/10.1002/adfm.201803665 D.K. Pradhan, S. Kumari et al., Magnetoelectric composites: applications, coupling mechanisms, and future directions. Nanomaterials. (2020). 10.(10).22.http://doi.org/10.3390/nano10102072 L.Y. Yang, X.Y. 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Zhang et al., High energy storage performance of all-inorganic flexible antiferroelectric-insulator multilayered thin films. ACS Appl. Mater. Interfaces. 14 (25), 28997–29006 (2022). http://doi.org/10.1021/acsami.2c05455 Additional Declarations Competing interest reported. Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper. Supplementary Files Supplementmaterials.docx Cite Share Download PDF Status: Published Journal Publication published 22 Jan, 2026 Read the published version in Journal of Materials Science: Materials in Electronics → Version 1 posted You are reading this latest preprint version Research Square lets you share your work early, gain feedback from the community, and start making changes to your manuscript prior to peer review in a journal. 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2","display":"","copyAsset":false,"role":"figure","size":634910,"visible":true,"origin":"","legend":"\u003cp\u003eCrystal structure and microscopic morphology of single and multilayer thin films. (a, c) XRD patterns of all films and (b, d) zoom-in images of (002) peak. (e) Cross-sectional TEM images of the (RAA)\u003csub\u003e2 \u003c/sub\u003emultilayer thin film, and (g, i) the SAED patterns of certain regions labeled white and orange, respectively.\u003c/p\u003e","description":"","filename":"floatimage2.png","url":"https://assets-eu.researchsquare.com/files/rs-7912657/v1/ccd55a9edd8416b8f539f093.png"},{"id":95861942,"identity":"0c855b57-5a6f-4970-9d18-b2ba89cc3dac","added_by":"auto","created_at":"2025-11-13 18:02:16","extension":"png","order_by":3,"title":"Figure 3","display":"","copyAsset":false,"role":"figure","size":138047,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cem\u003eP\u003c/em\u003e–\u003cem\u003eE \u003c/em\u003eand \u003cem\u003eI\u003c/em\u003e–\u003cem\u003eE\u003c/em\u003e curves of multilayer thin films with different stacking orders measured at 0.85 Mv cm\u003csup\u003e−1\u003c/sup\u003e.\u003c/p\u003e","description":"","filename":"floatimage3.png","url":"https://assets-eu.researchsquare.com/files/rs-7912657/v1/2013bf845e963d860f13715b.png"},{"id":96241477,"identity":"1b152419-84cb-4463-8262-5280da99fd17","added_by":"auto","created_at":"2025-11-19 07:10:46","extension":"png","order_by":4,"title":"Figure 4","display":"","copyAsset":false,"role":"figure","size":227630,"visible":true,"origin":"","legend":"\u003cp\u003e(a)-(d) Unipolar \u003cem\u003eP\u003c/em\u003e–\u003cem\u003eE \u003c/em\u003eloops of multilayer thin films with different stacking orders measured at their BDS, (e) \u003cem\u003eP\u003c/em\u003e\u003csub\u003emax\u003c/sub\u003e,\u003csub\u003e \u003c/sub\u003e\u003cem\u003eP\u003c/em\u003e\u003csub\u003er\u003c/sub\u003e, and their differences (Δ\u003cem\u003eP\u003c/em\u003e), (f) \u003cem\u003eW\u003c/em\u003e\u003csub\u003erec\u003c/sub\u003e and \u003cem\u003eη\u003c/em\u003e, (g) the Weibull distributions of BDS.\u003c/p\u003e","description":"","filename":"floatimage48.png","url":"https://assets-eu.researchsquare.com/files/rs-7912657/v1/8ae445fd14038184ad2b2117.png"},{"id":95861954,"identity":"b756e266-4f37-4ed1-b4ad-63cc466750b3","added_by":"auto","created_at":"2025-11-13 18:02:16","extension":"png","order_by":5,"title":"Figure 5","display":"","copyAsset":false,"role":"figure","size":237317,"visible":true,"origin":"","legend":"\u003cp\u003e(a)-(c) \u003cem\u003eP\u003c/em\u003e–\u003cem\u003eE\u003c/em\u003e curves and corresponding \u003cem\u003eI\u003c/em\u003e–\u003cem\u003eE \u003c/em\u003ecurves of multilayer thin films with different AFE layer thicknesses measured at 1.25, 0.85 and 0.625 Mv cm\u003csup\u003e-1\u003c/sup\u003e. (d) Unipolar \u003cem\u003eP\u003c/em\u003e–\u003cem\u003eE \u003c/em\u003eloops of multilayer thin films with different AFE layer thicknesses measured at their BDS, (e) \u003cem\u003eP\u003c/em\u003e\u003csub\u003emax\u003c/sub\u003e,\u003csub\u003e \u003c/sub\u003e\u003cem\u003eP\u003c/em\u003e\u003csub\u003er\u003c/sub\u003e, and their differences (Δ\u003cem\u003eP\u003c/em\u003e), (f) \u003cem\u003eW\u003c/em\u003e\u003csub\u003erec\u003c/sub\u003e and \u003cem\u003eη\u003c/em\u003e.\u003c/p\u003e","description":"","filename":"floatimage53.png","url":"https://assets-eu.researchsquare.com/files/rs-7912657/v1/1b08db62fcae9a13289a0e77.png"},{"id":96241415,"identity":"862e435e-7073-4146-944c-f52a3c69b700","added_by":"auto","created_at":"2025-11-19 07:10:41","extension":"png","order_by":6,"title":"Figure 6","display":"","copyAsset":false,"role":"figure","size":239531,"visible":true,"origin":"","legend":"\u003cp\u003eEnergy storage stability properties of the single and multilayer thin films. (a) Frequency reliability, (b) cycle stability, and (c) temperature stability of energy storage properties for representative (RA)\u003csub\u003e2 \u003c/sub\u003ethin films (d) Performance comparison of (RA)\u003csub\u003e2\u003c/sub\u003e with other films.\u003c/p\u003e","description":"","filename":"floatimage6.png","url":"https://assets-eu.researchsquare.com/files/rs-7912657/v1/1c5342a45e85cdcd60bfbe6b.png"},{"id":101151720,"identity":"7a6967b4-3b0c-4ade-9d8d-70ec087d8f66","added_by":"auto","created_at":"2026-01-26 16:03:00","extension":"pdf","order_by":0,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":2440244,"visible":true,"origin":"","legend":"","description":"","filename":"manuscript.pdf","url":"https://assets-eu.researchsquare.com/files/rs-7912657/v1/9f890bc0-f7e1-4c1c-9062-19bddb5ce172.pdf"},{"id":95861940,"identity":"281f6c87-4421-4732-9252-5cd925215ded","added_by":"auto","created_at":"2025-11-13 18:02:16","extension":"docx","order_by":0,"title":"","display":"","copyAsset":false,"role":"supplement","size":1574152,"visible":true,"origin":"","legend":"","description":"","filename":"Supplementmaterials.docx","url":"https://assets-eu.researchsquare.com/files/rs-7912657/v1/40fcd40831a61b45a0c1e000.docx"}],"financialInterests":"Competing interest reported. Declaration of Competing Interest\nThe authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.","formattedTitle":"Stacking pattern effect on the energy storage performance of PLZT-based relaxor- ferroelectric/antiferroelectric multilayer thin film capacitors prepared by sol-gel methods","fulltext":[{"header":"1. Introduction","content":"\u003cp\u003eDielectric thin films have great potential in micro-scale energy storage devices due to their ultrahigh power density, fast charge/discharge speed, and long lifespan [\u003cspan citationid=\"CR1\" class=\"CitationRef\"\u003e1\u003c/span\u003e]. To improve recoverable energy storage density (\u003cem\u003eW\u003c/em\u003e\u003csub\u003erec\u003c/sub\u003e) and the efficiency (\u003cem\u003eη\u003c/em\u003e), it is imperative to increase both the maximum polarization (\u003cem\u003eP\u003c/em\u003e\u003csub\u003emax\u003c/sub\u003e) and the electric breakdown strength (\u003cem\u003eE\u003c/em\u003e\u003csub\u003eb\u003c/sub\u003e), and reduce the remanent polarization (\u003cem\u003eP\u003c/em\u003e\u003csub\u003er\u003c/sub\u003e). Many strategies have been proposed, such as doping modifications, strain engineering, thickness optimization, and constructing of multilayers [\u003cspan citationid=\"CR2\" class=\"CitationRef\"\u003e2\u003c/span\u003e].\u003c/p\u003e\u003cp\u003eVarious multilayer thin film configurations consisting of ferroelectric (FE), relaxor ferroelectric (RFE), and antiferroelectric (AFE) thin films have been designed [\u003cspan citationid=\"CR1\" class=\"CitationRef\"\u003e1\u003c/span\u003e, \u003cspan additionalcitationids=\"CR4\" citationid=\"CR3\" class=\"CitationRef\"\u003e3\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e]. It has been reported that the (AFE/RFE)\u003csub\u003en\u003c/sub\u003e-type (PbZrO\u003csub\u003e3\u003c/sub\u003e/Pb\u003csub\u003e0.9\u003c/sub\u003eLa\u003csub\u003e0.1\u003c/sub\u003eZr\u003csub\u003e0.52\u003c/sub\u003eTi\u003csub\u003e0.48\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e)\u003csub\u003e8\u003c/sub\u003e multilayers prepared by laser pulsed deposition (PLD) exhibited an enhanced energy storage density with high efficiency (\u003cem\u003eW\u003c/em\u003e\u003csub\u003erec\u003c/sub\u003e of 128.4 J cm\u003csup\u003e\u0026minus;\u0026thinsp;3\u003c/sup\u003e and \u003cem\u003eη\u003c/em\u003e of 81.2% at the BDS of 4.2 MV cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e) due to the polarization coupling at the interfaces via epitaxial strains [\u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e]. However, such physical vapor deposition methods like PLD are not convenient for large-scale industrial production.\u003c/p\u003e\u003cp\u003eChemical methods like the sol-gel/spin coating method can easily prepare multilayer thin films with simple equipment at low cost [\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e]. Unlike the epitaxial multilayers prepared by PLD, the chemically prepared polycrystalline multilayers may benefit less from the interface strain coupling. Still, the interfaces contribute to the improvement in energy storage density. Such positive interface effect is attributed to the blocking of the growth and propagation of electrical trees [\u003cspan citationid=\"CR9\" class=\"CitationRef\"\u003e9\u003c/span\u003e]. However, the negative interface effect also exists where the lattice mismatch may induce a large number of defects at the interface regions, impairing BDS. Considering that both the positive and negative interface effects are closely related to the multilayer period and the thickness of individual layer, it is important to investigate their effects on the energy storage performances of dielectric multilayer thin films.\u003c/p\u003e\u003cp\u003eLanthanum doped lead zirconate titanate (PLZT) is one of the most studied dielectric materials [\u003cspan citationid=\"CR10\" class=\"CitationRef\"\u003e10\u003c/span\u003e]. According to its phase diagram, PLZT exhibits the FE feature at the titanate-rich region and the AFE feature at the zirconate-rich region [\u003cspan citationid=\"CR11\" class=\"CitationRef\"\u003e11\u003c/span\u003e]; whereas the dope of lanthanum is an effective approach to breaking the long-term ordering of electrical dipoles, stabilizing the AFE phase to the low-zirconate region or inducing the RFE phase in the FE region [\u003cspan additionalcitationids=\"CR13\" citationid=\"CR12\" class=\"CitationRef\"\u003e12\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR14\" class=\"CitationRef\"\u003e14\u003c/span\u003e]. The PLZT thin films with the RFE phase have been evidenced as excellent energy storage media with ultrahigh energy storage efficiencies due to its slim hysteresis loops (\u003cem\u003eP\u003c/em\u003e-\u003cem\u003eE\u003c/em\u003e loops) and low \u003cem\u003eP\u003c/em\u003e\u003csub\u003er\u003c/sub\u003e [\u003cspan citationid=\"CR15\" class=\"CitationRef\"\u003e15\u003c/span\u003e]. However, the relatively low \u003cem\u003eP\u003c/em\u003e\u003csub\u003emax\u003c/sub\u003e of RFE PLZT limits its maximum energy storage density. On the other hand, the AFE PLZT thin films show double \u003cem\u003eP\u003c/em\u003e-\u003cem\u003eE\u003c/em\u003e loops and almost zero \u003cem\u003eP\u003c/em\u003e\u003csub\u003er\u003c/sub\u003e value [\u003cspan citationid=\"CR16\" class=\"CitationRef\"\u003e16\u003c/span\u003e], making it favourable for energy storage applications, too. It has been reported that the PLZT multilayer thin films consisting of both AFE and RFE phases show better energy storage performances [\u003cspan citationid=\"CR17\" class=\"CitationRef\"\u003e17\u003c/span\u003e], where the stacking pattern is a key factor that affects the interface density. However, since the thickness of individual layer prepared by the sol-gel/spin coating method can hardly be adjusted, the thickness effect has rarely been investigated, though the ratio of the AFE phase to the entire multilayer thin film could significantly modify the shape of the \u003cem\u003eP\u003c/em\u003e-\u003cem\u003eE\u003c/em\u003e loops.\u003c/p\u003e\u003cp\u003eHerein, the PLZT multilayer thin films with different RFE/AFE stacking patterns were prepared by the sol-gel/spin-coating method. The thickness of AFE layers were adjusted by changing the stacking patterns, and the thickness effect on the energy storage performances of the multiplayer thin film was investigated. The BDS was enhanced due to the interface effect. As the result, the energy storage density of 26.28 J cm\u003csup\u003e\u0026minus;\u0026thinsp;3\u003c/sup\u003e was achieved in the designed PLZT multilayer thin film.\u003c/p\u003e"},{"header":"2. Experimental procedure","content":"\u003cp\u003eThe RFE-type (Pb\u003csub\u003e0.92\u003c/sub\u003eLa\u003csub\u003e0.08\u003c/sub\u003e)(Zr\u003csub\u003e0.65\u003c/sub\u003eTi\u003csub\u003e0.35\u003c/sub\u003e)O\u003csub\u003e3\u003c/sub\u003e (denoted as R) and AFE-type (Pb\u003csub\u003e0.98\u003c/sub\u003eLa\u003csub\u003e0.02\u003c/sub\u003e)(Zr\u003csub\u003e0.95\u003c/sub\u003eTi\u003csub\u003e0.05\u003c/sub\u003e)O\u003csub\u003e3\u003c/sub\u003e (denoted as A) were chosen as the RFE and AFE phases in the PLZT multilayer thin films, respectively. The PLZT multilayer thin films with various AFE/RFE stacking patterns were prepared on the Pt/Ti/SiO\u003csub\u003e2\u003c/sub\u003e/Si substrates by the sol-gel/spin-coating method. Initially, the raw materials were precisely weighed to match the atomic ratio requirements. To compensate for the loss of Pb during the heat treatment, an excess of 10% Pb was used in the precursor solution. Lead acetate trihydrate (PbC\u003csub\u003e4\u003c/sub\u003eH\u003csub\u003e6\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e\u0026middot;3H\u003csub\u003e2\u003c/sub\u003eO, 99.99%, Aladdin) and lanthanum nitrate hexahydrate (LaN\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e9\u003c/sub\u003e\u0026middot;6H\u003csub\u003e2\u003c/sub\u003eO, 99%, Aladdin) were stirred in 2-Methoxyethanol (C\u003csub\u003e3\u003c/sub\u003eH\u003csub\u003e8\u003c/sub\u003eO\u003csub\u003e2\u003c/sub\u003e, AR, Aladdin) for 2 h at 70\u0026deg;C, forming Solution A. Simultaneously, zirconium propoxide (C\u003csub\u003e12\u003c/sub\u003eH\u003csub\u003e28\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003eZr, 70 wt.%, Aladdin) and titanium butoxide (C\u003csub\u003e16\u003c/sub\u003eH\u003csub\u003e36\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003eTi, \u0026ge; 99.0%, Aladdin) were stirred in 2-Methoxyethanol for 1 h at room temperature. An appropriate amount of acetylacetone (C\u003csub\u003e5\u003c/sub\u003eH\u003csub\u003e8\u003c/sub\u003eO\u003csub\u003e2\u003c/sub\u003e, 99%, Aladdin) and formamide (CH\u003csub\u003e3\u003c/sub\u003eNO, 99%, Aladdin) were added as chelating agents to stabilize the solution, forming Solution B. Then, Solution B was mixed with Solution A, and the pH was adjusted by adding a certain amount of glacial acetic acid (CH\u003csub\u003e3\u003c/sub\u003eCOOH, AR, Sinopharm Chemical Reagent Co.), followed by continuous stirring at 70\u0026deg;C for 2 h to obtain precursor sols. The precursor solution was aged for 48 h. Then, each layer was spin-coated on the substrate at 4000 rpm for 30 s. The as-grown films were heated on a hot plate at 100 ℃ for 2 min and pyrolyzed in a tube furnace at 450 ℃ for 5 min. Such procedures were repeated several times using different precursors to construct desired stacking patterns. The stacking orders of multilayers were R/A/R/A/R/A, R/A/R/A, R/A/A/R/A/A, and R/A/A/A/R/A/A/A, denoted as (RA)\u003csub\u003e3\u003c/sub\u003e, (RA)\u003csub\u003e2\u003c/sub\u003e, (RAA)\u003csub\u003e2\u003c/sub\u003e, and (RAAA)\u003csub\u003e2\u003c/sub\u003e, respectively. For comparison, the pure RFE (6R layers, R\u003csub\u003e6\u003c/sub\u003e) and AFE thin films (6A layers, A\u003csub\u003e6\u003c/sub\u003e) were also prepared. The schematics of all the above multilayer thin film structures are shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003e. Finally, the thin films were crystallized using a rapid thermal annealing furnace at 700 ℃ for 30 min with heating rate was 15 ℃/s.\u003c/p\u003e\u003cp\u003e\u003c/p\u003e\u003cp\u003eThe crystal structure of the multilayer thin films was determined using X-ray diffraction (XRD, Ultima III, Rigaku) with a Cu K\u003csub\u003eα\u003c/sub\u003e radiation. A pseudocubic (PC) index was used when discussing crystal structures in this text. The local crystal structure and domain distribution of the (RAA)\u003csub\u003e2\u003c/sub\u003e multilayer thin film was measured using transmission electron microscopy (TEM, Talos F200I, FEI) with a working voltage of 200 kV. The TEM sample was prepared by the focusing ion beam (FIB, Helios G4 CX, FEI). The thickness of thin films was measured using field-emission scanning electron microscopy (FESEM, Supra 55, Carl Zeiss). The surface morphology was observed using atomic force microscopy (AFM, MFP-3D, Asylum Research). The Raman spectra were measured using the Raman spectrometer (DXR-2Xi, Thermo Fisher Scientific) with a laser excitation at 532 nm wavelength.\u003c/p\u003e\u003cp\u003eThe polarization (\u003cem\u003eP\u0026ndash;E\u003c/em\u003e) and current (\u003cem\u003eI\u0026ndash;E\u003c/em\u003e) hysteresis loops of thin films were measured using a ferroelectric analyzer (AIX ACT, TF2000) at 1 kHz, from which the \u003cem\u003eW\u003c/em\u003e\u003csub\u003erec\u003c/sub\u003e and \u003cem\u003eη\u003c/em\u003e were calculated by the following equations:\u003cdiv id=\"Equ1\" class=\"Equation\"\u003e\u003cdiv format=\"TEX\" class=\"mathdisplay\" id=\"FileID_Equ1\" name=\"EquationSource\"\u003e\n$$\\:{W}_{\\text{t}\\text{o}\\text{l}}=\\:{\\int\\:}_{0}^{{P}_{max}}EdP={W}_{rec}+\\:{W}_{\\text{l}\\text{o}\\text{s}\\text{s}}$$\u003c/div\u003e\u003cdiv class=\"EquationNumber\"\u003e1\u003c/div\u003e\u003c/div\u003e\u003cdiv id=\"Equ2\" class=\"Equation\"\u003e\u003cdiv format=\"TEX\" class=\"mathdisplay\" id=\"FileID_Equ2\" name=\"EquationSource\"\u003e\n$$\\:{W}_{rec}=\\:{\\int\\:}_{{P}_{r}}^{{P}_{max}}EdP$$\u003c/div\u003e\u003cdiv class=\"EquationNumber\"\u003e2\u003c/div\u003e\u003c/div\u003e\u003cdiv id=\"Equ3\" class=\"Equation\"\u003e\u003cdiv format=\"TEX\" class=\"mathdisplay\" id=\"FileID_Equ3\" name=\"EquationSource\"\u003e\n$$\\:\\eta\\:=\\:\\frac{{W}_{rec}}{{W}_{tol}}\\:\\times\\:100\\%$$\u003c/div\u003e\u003cdiv class=\"EquationNumber\"\u003e3\u003c/div\u003e\u003c/div\u003e\u003c/p\u003e\u003cp\u003ewhere \u003cem\u003eP\u003c/em\u003e\u003csub\u003emax\u003c/sub\u003e is the maximum polarization, \u003cem\u003eP\u003c/em\u003e\u003csub\u003er\u003c/sub\u003e is the remanent polarization, \u003cem\u003eE\u003c/em\u003e is the applied electric field, \u003cem\u003eP\u003c/em\u003e is the polarization, and \u003cem\u003eW\u003c/em\u003e\u003csub\u003eloss\u003c/sub\u003e is the energy loss density. For the performance stability measurements, \u003cem\u003eP\u0026ndash;E\u003c/em\u003e loops of the (RA)\u003csub\u003e2\u003c/sub\u003e multilayer thin film were tested up to 10\u003csup\u003e6\u003c/sup\u003e cycles with pulses of 0.5 kHz \u0026minus;\u0026thinsp;2 kHz using 1.25 MV cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e as the switching field. For the thermostability, the \u003cem\u003eP\u0026ndash;E\u003c/em\u003e loops of the same sample were measured with temperature increasing to 170 ℃.\u003c/p\u003e"},{"header":"3. Results","content":"\u003cdiv id=\"Sec4\" class=\"Section2\"\u003e\u003ch2\u003e3.1. The morphology and structure of PLZT multilayer thin films\u003c/h2\u003e\u003cp\u003eThe AFM images in \u003cb\u003eFigure \u003cspan refid=\"MOESM1\" class=\"InternalRef\"\u003eS1\u003c/span\u003e\u003c/b\u003e exhibit smooth surfaces for all the samples with the roughness less than 3.5 nm. The cross-sectional SEM images in \u003cb\u003eFigure S2\u003c/b\u003e suggest the thickness of different samples is between 247 nm (4 layers) and 497 nm (8 layers), corresponding to a thickness of 65 nm for each individual layer.\u003c/p\u003e\u003cp\u003eThe XRD patterns in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ea and \u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ec suggest that all the PLZT multilayer thin films exhibit the pure perovskite phase. In order to further analyse the effect of different stacking orders on the structure, a magnified view around the (002) peaks are presented in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003eb, where significant shifts are observed. The (002) peak of A\u003csub\u003e6\u003c/sub\u003e is located at 2θ\u0026thinsp;=\u0026thinsp;43.87 \u0026deg; (corresponding to a lattice parameter c of 0.4124 nm), while that of R\u003csub\u003e6\u003c/sub\u003e is located at 2θ\u0026thinsp;=\u0026thinsp;44.34 \u0026deg; (c\u0026thinsp;=\u0026thinsp;0.4082 nm). For multilayers, the (002) peak of (RAA)\u003csub\u003e2\u003c/sub\u003e film is located at 2θ\u0026thinsp;=\u0026thinsp;43.90 \u0026deg; (c\u0026thinsp;=\u0026thinsp;0.4122 nm), and that of (RA)\u003csub\u003e3\u003c/sub\u003e film is located at 2θ\u0026thinsp;=\u0026thinsp;43.97 \u0026deg; (c\u0026thinsp;=\u0026thinsp;0.4116 nm). Such shift is attributed to the lattice mismatch between the R and A phases (1.02%). In Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ed, the multilayer films with the same stacking order but different AFE layer thicknesses exhibit almost the same (002) peak location ((RA)\u003csub\u003e2\u003c/sub\u003e: 43.92 \u0026deg;, (RAA)\u003csub\u003e2\u003c/sub\u003e: 43.90 \u0026deg;, (RAAA)\u003csub\u003e2\u003c/sub\u003e: 43.89 \u0026deg;), which corresponds to a 0.05% fluctuation in the lattice constant. However, the decrease of the full width half maximum (FWHM) with the decreasing thickness suggests that the internal stress inside the multilayer thin films is increased due to the lattice mismatch.\u003c/p\u003e\u003cp\u003eFigure \u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ee shows the cross-sectional TEM image of the (RAA)\u003csub\u003e2\u003c/sub\u003e multilayer thin film, where the dense multilayer structure with the distinguishable R/A interfaces is observed. Specifically, in the R layer (Position ① in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ee), nanodomains with a size of 10 nm are observed, evidencing the existence of polar nanoregions (PNRs) for RFEs. Figure\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ef and \u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003eg show the high-resolution TEM (HRTEM) images and the corresponding selected area electron diffraction (SAED) patterns of the R layer, respectively, where only the lattice reflections are observed. Meanwhile, the SAED pattern \u003cb\u003e(\u003c/b\u003eFig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ei) of the A layer (Position ② in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ee) exhibits the (011) superlattice reflections, which represents a periodic antiparallel arrangement of Pb\u003csup\u003e2+\u003c/sup\u003e ions and reveals the AFE nature of the A layer[\u003cspan citationid=\"CR18\" class=\"CitationRef\"\u003e18\u003c/span\u003e, \u003cspan citationid=\"CR19\" class=\"CitationRef\"\u003e19\u003c/span\u003e].\u003c/p\u003e\u003cp\u003e\u003c/p\u003e\u003cp\u003eThe Raman spectra of the multilayer thin films with different stacking orders are plotted in \u003cb\u003eFigure S3a\u003c/b\u003e in the Supplementary Material. The Raman spectra exhibit characteristic peaks at 129 cm⁻\u0026sup1;, 233 cm\u003csup\u003e-1\u003c/sup\u003e, 341 cm⁻\u0026sup1;, and 525 cm⁻\u0026sup1;, corresponding to Pb-(ZrO₃) lattice mode, Zr-O bending mode, ZrO₃ twisting mode, and Zr-O/Ti-O bending modes, respectively[\u003cspan citationid=\"CR20\" class=\"CitationRef\"\u003e20\u003c/span\u003e]. Among them, the Pb-(ZrO\u003csub\u003e3\u003c/sub\u003e) lattice mode is related to the AFE orthorhombic phase, whose disappearance in the samples other than the A\u003csub\u003e6\u003c/sub\u003e thin film indicates the suppression of AFE phase by introducing the RFE layer [\u003cspan citationid=\"CR16\" class=\"CitationRef\"\u003e16\u003c/span\u003e, \u003cspan citationid=\"CR21\" class=\"CitationRef\"\u003e21\u003c/span\u003e]. Figure S3b shows the Raman spectra of multilayer thin films with different thicknesses of the AFE layers. With the increase of thickness, the Raman peaks at both 233 cm\u003csup\u003e-1\u003c/sup\u003e and 525 cm\u003csup\u003e-1\u003c/sup\u003e shift slightly towards the higher wave number direction (\u003cem\u003ei.e.\u003c/em\u003e, the peak position of the pure R\u003csub\u003e6\u003c/sub\u003e phase), which associates with the enhanced octahedral torsion and structural distortion, indicating that the structure of multilayer thin films progressively transforms into a RFE-like mode [\u003cspan citationid=\"CR22\" class=\"CitationRef\"\u003e22\u003c/span\u003e].\u003c/p\u003e\u003c/div\u003e\u003cdiv id=\"Sec5\" class=\"Section2\"\u003e\u003ch2\u003e3.2. The effect of the stacking order on the energy storage performance\u003c/h2\u003e\u003cp\u003eThe \u003cem\u003eP\u0026ndash;E\u003c/em\u003e and \u003cem\u003eI\u0026ndash;E\u003c/em\u003e curves of the thin films with different stacking orders are measured at 0.85 MV cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e and 1 kHz, as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003e. A\u003csub\u003e6\u003c/sub\u003e exhibits a double \u003cem\u003eP\u0026ndash;E\u003c/em\u003e loop with four sharp current-switching peaks in the \u003cem\u003eI\u0026ndash;E\u003c/em\u003e curve, evidencing the reversible AFE-FE phase transition. For comparison, R\u003csub\u003e6\u003c/sub\u003e shows a typical RFE-like slender \u003cem\u003eP\u0026ndash;E\u003c/em\u003e loop. Interestingly, (RA)\u003csub\u003e3\u003c/sub\u003e and (RAA)\u003csub\u003e2\u003c/sub\u003e multilayer thin films exhibit different dielectric features. The AFE-like switching behavior is only observed in the (RA)\u003csub\u003e3\u003c/sub\u003e multilayer thin film, evidenced by the corresponding \u003cem\u003eI\u0026ndash;E\u003c/em\u003e curve, whereas the (RAA)\u003csub\u003e2\u003c/sub\u003e one exhibits a RFE-type \u003cem\u003eP\u0026ndash;E\u003c/em\u003e loop. Such difference in dielectric features is attributed to the different AFE/RFE stacking orders that may affect the interface strain condition and the thin film crystallinity inside each layer [\u003cspan citationid=\"CR23\" class=\"CitationRef\"\u003e23\u003c/span\u003e].\u003c/p\u003e\u003cp\u003eThe unipolar \u003cem\u003eP\u0026ndash;E\u003c/em\u003e loops of the multilayer thin films at their BDS are shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ea-\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ed. Figure\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ee shows that \u003cem\u003eP\u003c/em\u003e\u003csub\u003e\u003cem\u003emax\u003c/em\u003e\u003c/sub\u003e of the (RAA)\u003csub\u003e2\u003c/sub\u003e and (RA)\u003csub\u003e3\u003c/sub\u003e multilayer thin films are 57.12 \u0026micro;C cm\u003csup\u003e\u0026minus;\u0026thinsp;2\u003c/sup\u003e at 2.72 MV cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e and 44.8 \u0026micro;C cm\u003csup\u003e\u0026minus;\u0026thinsp;2\u003c/sup\u003e at 2.54 MV cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, respectively, which are larger than that of the pure A\u003csub\u003e6\u003c/sub\u003e thin films. The introduction of the RFE layers leads to an enhanced \u003cem\u003eP\u003c/em\u003e\u003csub\u003e\u003cem\u003emax\u003c/em\u003e\u003c/sub\u003e value in the multilayer thin film [\u003cspan citationid=\"CR22\" class=\"CitationRef\"\u003e22\u003c/span\u003e]. A near-zero \u003cem\u003eP\u003c/em\u003e\u003csub\u003er\u003c/sub\u003e value is detected for A\u003csub\u003e6\u003c/sub\u003e and R\u003csub\u003e6\u003c/sub\u003e, whereas the multilayer thin films exhibit nonnegligible \u003cem\u003eP\u003c/em\u003e\u003csub\u003er\u003c/sub\u003e. It is due to the inhibition of domain switching as the defect density is increased by inducing the AFE/RFE interfaces. Since the (RA)\u003csub\u003e3\u003c/sub\u003e multilayer thin film has more R/A interfaces than the (RAA)\u003csub\u003e2\u003c/sub\u003e one, the \u003cem\u003eΔP\u003c/em\u003e of (RA)\u003csub\u003e3\u003c/sub\u003e is smaller than that of (RAA)\u003csub\u003e2\u003c/sub\u003e. Figure\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ef shows that the \u003cem\u003eW\u003c/em\u003e\u003csub\u003e\u003cem\u003erec\u003c/em\u003e\u003c/sub\u003e of A\u003csub\u003e6\u003c/sub\u003e, R\u003csub\u003e6\u003c/sub\u003e, (RA)\u003csub\u003e3\u003c/sub\u003e, and (RAA)\u003csub\u003e2\u003c/sub\u003e samples are 18.8 J cm\u003csup\u003e\u0026minus;\u0026thinsp;3\u003c/sup\u003e,16.2 J cm\u003csup\u003e\u0026minus;\u0026thinsp;3\u003c/sup\u003e,11.96 J cm\u003csup\u003e\u0026minus;\u0026thinsp;3\u003c/sup\u003e and 18.74 J cm\u003csup\u003e\u0026minus;\u0026thinsp;3\u003c/sup\u003e, respectively, and their \u003cem\u003eη\u003c/em\u003e are 48%, 48.66%, 19.3%, 41.09%, respectively. The fitting BDS from the Weibull distributions for A\u003csub\u003e6\u003c/sub\u003e, R\u003csub\u003e6\u003c/sub\u003e, (RA)\u003csub\u003e3\u003c/sub\u003e and (RAA)\u003csub\u003e2\u003c/sub\u003e thin films are 1.93, 1.803, 2.54, and 2.72 MV cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, respectively, as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003eg, in consistence with the results in Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ea-\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ed. In sum, the multilayer thin films with three R/A interfaces show better energy storage performances than those with five R/A interfaces.\u003c/p\u003e\u003cp\u003e\u003c/p\u003e\u003cp\u003e\u003c/p\u003e\u003c/div\u003e\u003cdiv id=\"Sec6\" class=\"Section2\"\u003e\u003ch2\u003e3.3. The effect of the thickness on energy storage performance\u003c/h2\u003e\u003cp\u003eNext, the energy storage properties of (RA)\u003csub\u003e2\u003c/sub\u003e, (RAA)\u003csub\u003e2\u003c/sub\u003e, and (RAAA)\u003csub\u003e2\u003c/sub\u003e multilayer thin films were compared. Note that these three samples have the same interface number but different AFE layer thicknesses. As shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ea\u003cb\u003e-Figure 5c\u003c/b\u003e, (RA)\u003csub\u003e2\u003c/sub\u003e exhibits thinnest \u003cem\u003eP\u003c/em\u003e\u0026ndash;\u003cem\u003eE\u003c/em\u003e loops with four obvious peaks in the \u003cem\u003eI\u003c/em\u003e\u0026ndash;\u003cem\u003eE\u003c/em\u003e loops, suggesting a relaxor AFE (RAFE) feature. Such results indicate that the (RA)\u003csub\u003e3\u003c/sub\u003e multilayer films might have also belonged to the RAFE phase because they have similar stacking orders. However, the negative interface effect induces defects that \u0026ldquo;broaden\u0026rdquo; the \u003cem\u003eP\u003c/em\u003e\u0026ndash;\u003cem\u003eE\u003c/em\u003e loops (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ec).\u003c/p\u003e\u003cp\u003eWith the increasing thickness of AFE layers, the multilayer thin films trend to exhibit the RFE feature in (RAA)\u003csub\u003e2\u003c/sub\u003e and the FE one in (RAAA)\u003csub\u003e2\u003c/sub\u003e. As the result, the \u003cem\u003eP\u003c/em\u003e\u003csub\u003er\u003c/sub\u003e value is gradually increased. Figure\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ed illustrates the unipolar \u003cem\u003eP\u003c/em\u003e\u0026ndash;\u003cem\u003eE\u003c/em\u003e loops of films with different AFE layer thicknesses at \u003cem\u003eE\u003c/em\u003e\u003csub\u003eb\u003c/sub\u003e. With the increase of AFE layer thickness, \u003cem\u003eE\u003c/em\u003e\u003csub\u003eb\u003c/sub\u003e decreases. Such phenomena are attributed to the thicker thickness that weaken the positive interfacial effect[\u003cspan citationid=\"CR24\" class=\"CitationRef\"\u003e24\u003c/span\u003e]. Therefore, the good energy storage performance in the (RFE/AFE)\u003csub\u003e2\u003c/sub\u003e-type multilayers might probably be attributed to the positive interface effect.\u003c/p\u003e\u003cp\u003eAs shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ee, with the increase of AFE layer thickness, the \u003cem\u003eP\u003c/em\u003e\u003csub\u003e\u003cem\u003emax\u003c/em\u003e\u003c/sub\u003e changes little, \u003cem\u003eΔP\u003c/em\u003e first increases then decreases. The \u003cem\u003eW\u003c/em\u003e\u003csub\u003erec\u003c/sub\u003e of (RA)\u003csub\u003e2\u003c/sub\u003e, (RAA)\u003csub\u003e2\u003c/sub\u003e and (RAAA)\u003csub\u003e2\u003c/sub\u003e multilayer thin films is 26.28 J cm\u003csup\u003e\u0026minus;\u0026thinsp;3\u003c/sup\u003e, 18.74 J cm\u003csup\u003e\u0026minus;\u0026thinsp;3\u003c/sup\u003e and 17.17 J cm\u003csup\u003e\u0026minus;\u0026thinsp;3\u003c/sup\u003e, respectively, the corresponding \u003cem\u003eη\u003c/em\u003e is 49.78%, 41.09% and 58.86%, respectively, as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ef. Compared to the A\u003csub\u003e6\u003c/sub\u003e AFE thin films, the \u003cem\u003eW\u003c/em\u003e\u003csub\u003erec\u003c/sub\u003e of (RA)\u003csub\u003e2\u003c/sub\u003e is improves by 7.48 J cm\u003csup\u003e\u0026minus;\u0026thinsp;3\u003c/sup\u003e.\u003c/p\u003e\u003cp\u003e\u003c/p\u003e\u003cp\u003e\u003c/p\u003e\u003cp\u003eFor dielectric energy storage materials, reliability and stability is the key factors to evaluate the performance. Figure\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e6\u003c/span\u003e shows the energy storage reliability of (RA)\u003csub\u003e2\u003c/sub\u003e multilayer thin films at various frequencies, temperature, and cycles, respectively. The\u003c/p\u003e\u003cp\u003e(RA)\u003csub\u003e2\u003c/sub\u003e multilayer thin films have excellent frequency stability in the range of 0.5 kHz to 2 kHz, good temperature stability up to 170℃, and cycling reliability up to 10\u003csup\u003e6\u003c/sup\u003e cycles, ensuring the (RA)\u003csub\u003e2\u003c/sub\u003e multilayer thin film a promising candidate for energy storage capacitors.\u003c/p\u003e\u003c/div\u003e"},{"header":"4. Discussion","content":"\u003cp\u003ePublications have reported that the RFE PLZT (8/65/35) and the AFE PLZT(2/95/5) exhibit a rhombohedral structure and an orthorhombic structure, respectively[\u003cspan citationid=\"CR25\" class=\"CitationRef\"\u003e25\u003c/span\u003e]. The XRD patterns in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003e confirm such difference in structure. More importantly, all the multilayer thin films with various stacking patterns (either different stacking orders or different AFE layer thicknesses) exhibit a similar lattice constant value with the AFE A\u003csub\u003e6\u003c/sub\u003e sample (check Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003eb and \u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ed), indicating the AFE orthorhombic phase (AFE\u003csub\u003eO\u003c/sub\u003e) is dominating in all these multilayer thin films through they have several RFE layers inside.\u003c/p\u003e\u003cp\u003eHowever, the \u003cem\u003eP\u003c/em\u003e\u0026ndash;\u003cem\u003eE\u003c/em\u003e curves and corresponding \u003cem\u003eI\u003c/em\u003e\u0026ndash;\u003cem\u003eE\u003c/em\u003e curves in Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003e and Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003e indicate diverse dielectric features in the multilayer thin films with different stacking patterns. In detail, (RA)\u003csub\u003e3\u003c/sub\u003e, (RA)\u003csub\u003e2\u003c/sub\u003e, (RAA)\u003csub\u003e2\u003c/sub\u003e, and (RAAA)\u003csub\u003e2\u003c/sub\u003e show the AFE, RAFE, RFE, and FE phases, respectively. Among them, the (RA)\u003csub\u003e3\u003c/sub\u003e multilayer film might have also belonged to the RAFE phase because it has a similar stacking order with (RA)\u003csub\u003e2\u003c/sub\u003e. However, the negative interface effect induces defects that \u0026ldquo;broaden\u0026rdquo; the \u003cem\u003eP\u003c/em\u003e\u0026ndash;\u003cem\u003eE\u003c/em\u003e loops (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ec).\u003c/p\u003e\u003cp\u003eAdditionally, please note that the superlattice diffraction pattern in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ei evidences the existence of AFE phase in the (RAA)\u003csub\u003e2\u003c/sub\u003e multilayer thin film. The contradictory results between the SAED pattern and dielectric tests indicate the significant difference between the apparent and the local dielectric features in the (RAA)\u003csub\u003e2\u003c/sub\u003e multilayer thin film. Besides, it is interesting to find a FE feature in the multilayer thin film with the thickest AFE layers, where the reason needs further investigation.\u003c/p\u003e\u003cp\u003eAccording to the above discussion, although different multilayer thin films exhibit similar apparent crystal structure, their dielectric features are diverse, leading to different energy storage performances. Amongst them, (RA)\u003csub\u003e2\u003c/sub\u003e shows the best energy storage performance with \u003cem\u003eW\u003c/em\u003e\u003csub\u003erec\u003c/sub\u003e of 26.28 J cm\u003csup\u003e-3\u003c/sup\u003e and \u003cem\u003eη\u003c/em\u003e of 49.78%. The energy storage properties of multilayer thin films depend on \u003cem\u003eP\u003c/em\u003e\u003csub\u003emax\u003c/sub\u003e, \u003cem\u003eP\u003c/em\u003e\u003csub\u003er\u003c/sub\u003e, \u003cem\u003eE\u003c/em\u003e\u003csub\u003eA\u003c/sub\u003e, \u003cem\u003eE\u003c/em\u003e\u003csub\u003eF\u003c/sub\u003e, and \u003cem\u003eE\u003c/em\u003e\u003csub\u003eb\u003c/sub\u003e of samples, which is determined by the stacking patterns based on the interlayer coupling effect [\u003cspan citationid=\"CR26\" class=\"CitationRef\"\u003e26\u003c/span\u003e, \u003cspan citationid=\"CR27\" class=\"CitationRef\"\u003e27\u003c/span\u003e]. By modifying the stacking patterns, it is possible to construct various heterogeneous interface conditions in the multilayer thin films that may thus influence the energy storage performance in a positive or negative way[\u003cspan additionalcitationids=\"CR29\" citationid=\"CR28\" class=\"CitationRef\"\u003e28\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR30\" class=\"CitationRef\"\u003e30\u003c/span\u003e].\u003c/p\u003e\u003cp\u003eFirst, the interfacial blocking effect serves as a critical barrier against the growth and spread of electrical trees [\u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e, \u003cspan citationid=\"CR31\" class=\"CitationRef\"\u003e31\u003c/span\u003e]. Thus, a larger interface density could effectively enhance \u003cem\u003eE\u003c/em\u003e\u003csub\u003eb\u003c/sub\u003e (check Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ea-\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ed) and make positive contribution to the energy storage performance. However, the lattice mismatch between R and A phases induces significant interfacial stress [\u003cspan citationid=\"CR32\" class=\"CitationRef\"\u003e32\u003c/span\u003e]. Thus, the larger interface density would result in more defects at the interfaces region that promotes the generation of leakage currents (check the \u003cem\u003eP\u003c/em\u003e\u0026ndash;\u003cem\u003eE\u003c/em\u003e loops in Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003e), negatively affecting energy storage efficiency. As the result, it is a trade-off to design modest interface density to improve energy storage performance. As illustrated in Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003e, (RA)\u003csub\u003e3\u003c/sub\u003e contains two additional R/A interfaces compared to (RAA)\u003csub\u003e2\u003c/sub\u003e, leading to an increased energy loss density but the similar \u003cem\u003eE\u003c/em\u003e\u003csub\u003eb\u003c/sub\u003e, and thus poorer energy storage performance (check Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003e\u003cb\u003e)\u003c/b\u003e. Note that the interface stress effect is correlated to the fabrication methods. Some physical vapor deposition methods like PLD may induce a large amount of epitaxial stress (although some literature reported that such stress may enhance \u003cem\u003eP\u003c/em\u003e\u003csub\u003emax\u003c/sub\u003e)[\u003cspan citationid=\"CR33\" class=\"CitationRef\"\u003e33\u003c/span\u003e], whereas the chemical solution method like sol-gel/spin-coating could reduce the interfacial stress effect by the proper annealing process[\u003cspan citationid=\"CR34\" class=\"CitationRef\"\u003e34\u003c/span\u003e, \u003cspan citationid=\"CR35\" class=\"CitationRef\"\u003e35\u003c/span\u003e].\u003c/p\u003e\u003cp\u003eSecond, the thickness effect may also influence energy storage performance. Generally, reducing the thickness may impair the crystallinity of layers and increase the defects inside, increasing the energy loss density. However, such negative effects have a critical thickness (usually several tens of nanometers[\u003cspan citationid=\"CR36\" class=\"CitationRef\"\u003e36\u003c/span\u003e, \u003cspan citationid=\"CR37\" class=\"CitationRef\"\u003e37\u003c/span\u003e]) and are affected by the interfacial condition. In our cases, increasing the thickness of AFE layer (without changing the stacking orders) indeed decreases the energy loss density and improves the energy storage efficiency. However, the dielectric features of multilayer thin films have also changed, which leads to a decrease in energy storage density with increasing AFE layer thickness (check Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ed). The AFE phase thickness is controlled by stacking different numbers of AFE layers (65 nm per layer). Thus, the fact that the dielectric features would change from RAFE to FE phases indicates that the A/A interface condition also affects the dielectric behaviors. The lattice mismatch at the A/A interfaces caused by multiple spin-coating deposition sequences may also induce defects that could generate leakage current and might inhibit AFE-FE phase transition in a worse situation[\u003cspan citationid=\"CR38\" class=\"CitationRef\"\u003e38\u003c/span\u003e]. A layer-by-layer annealing approach may weaken the effect of such A/A lattice mismatch, but it is much more time-consuming and energy-costing.\u003c/p\u003e\u003cp\u003eAs shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e6\u003c/span\u003ed and Table\u0026nbsp;\u003cspan refid=\"Tab1\" class=\"InternalRef\"\u003e1\u003c/span\u003e, the (RA)\u003csub\u003e2\u003c/sub\u003e multilayer film has superior \u003cem\u003eE\u003c/em\u003e\u003csub\u003eb\u003c/sub\u003e and thus \u003cem\u003eW\u003c/em\u003e\u003csub\u003erec\u003c/sub\u003e, in comparison with other PZ-based FE/AFE multilayer thin films.\u003c/p\u003e\u003cp\u003e\u003cdiv class=\"gridtable\"\u003e\u003ctable float=\"Yes\" id=\"Tab1\" border=\"1\"\u003e\u003ccaption language=\"En\"\u003e\u003cdiv class=\"CaptionNumber\"\u003eTable 1\u003c/div\u003e\u003cdiv class=\"CaptionContent\"\u003e\u003cp\u003esummarizes the energy storage property densities of (RA)\u003csub\u003e2\u003c/sub\u003e multilayers and other AFE, RFE, and FE/AFE multilayer films.\u003c/p\u003e\u003c/div\u003e\u003c/caption\u003e\u003ccolgroup cols=\"7\"\u003e\u003cdiv align=\"left\" class=\"colspec\" colname=\"c1\" colnum=\"1\"\u003e\u003c/div\u003e\u003cdiv align=\"left\" class=\"colspec\" colname=\"c2\" colnum=\"2\"\u003e\u003c/div\u003e\u003cdiv align=\"left\" class=\"colspec\" colname=\"c3\" colnum=\"3\"\u003e\u003c/div\u003e\u003cdiv align=\"left\" class=\"colspec\" colname=\"c4\" colnum=\"4\"\u003e\u003c/div\u003e\u003cdiv align=\"left\" class=\"colspec\" colname=\"c5\" colnum=\"5\"\u003e\u003c/div\u003e\u003cdiv align=\"left\" class=\"colspec\" colname=\"c6\" colnum=\"6\"\u003e\u003c/div\u003e\u003cdiv align=\"left\" class=\"colspec\" colname=\"c7\" colnum=\"7\"\u003e\u003c/div\u003e\u003cthead\u003e\u003ctr\u003e\u003cth align=\"left\" colname=\"c1\"\u003e\u003cp\u003eRef.\u003c/p\u003e\u003c/th\u003e\u003cth align=\"left\" colname=\"c2\"\u003e\u003cp\u003e\u003cem\u003eW\u003c/em\u003e\u003csub\u003e\u003cem\u003erec\u003c/em\u003e\u003c/sub\u003e\u003c/p\u003e\u003cp\u003e(J cm\u003csup\u003e-3\u003c/sup\u003e)\u003c/p\u003e\u003c/th\u003e\u003cth align=\"left\" colname=\"c3\"\u003e\u003cp\u003e\u003cem\u003eη\u003c/em\u003e (%)\u003c/p\u003e\u003c/th\u003e\u003cth align=\"left\" colname=\"c4\"\u003e\u003cp\u003e\u003cem\u003eE\u003c/em\u003e (MV cm\u003csup\u003e-1\u003c/sup\u003e)\u003c/p\u003e\u003c/th\u003e\u003cth align=\"left\" colname=\"c5\"\u003e\u003cp\u003eMaterials\u003c/p\u003e\u003c/th\u003e\u003cth align=\"left\" colname=\"c6\"\u003e\u003cp\u003eTypes\u003c/p\u003e\u003c/th\u003e\u003cth align=\"left\" colname=\"c7\"\u003e\u003cp\u003ePreparation technique\u003c/p\u003e\u003c/th\u003e\u003c/tr\u003e\u003c/thead\u003e\u003ctbody\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003eThis work\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c2\"\u003e\u003cp\u003e26.28\u003c/p\u003e\u003cp\u003e9.59\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c3\"\u003e\u003cp\u003e49.28\u003c/p\u003e\u003cp\u003e62.25\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c4\"\u003e\u003cp\u003e3.19\u003c/p\u003e\u003cp\u003e1.25\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c5\"\u003e\u003cp\u003ePLZT\u003c/p\u003e\u003cp\u003ePLZT\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c6\"\u003e\u003cp\u003eAFE/RFE\u003c/p\u003e\u003cp\u003eAFE/RFE\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c7\"\u003e\u003cp\u003eSol-Gel\u003c/p\u003e\u003cp\u003eSol-Gel\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003eSheng Tong et al[\u003cspan citationid=\"CR39\" class=\"CitationRef\"\u003e39\u003c/span\u003e]\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c2\"\u003e\u003cp\u003e22\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c3\"\u003e\u003cp\u003e77\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c4\"\u003e\u003cp\u003e1.6\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c5\"\u003e\u003cp\u003ePLZT/LNO\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c6\"\u003e\u003cp\u003eRFE\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c7\"\u003e\u003cp\u003eSol-Gel\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003eNgo Duc Quan et al[\u003cspan citationid=\"CR40\" class=\"CitationRef\"\u003e40\u003c/span\u003e]\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c2\"\u003e\u003cp\u003e8.1\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c3\"\u003e\u003cp\u003e56.2\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c4\"\u003e\u003cp\u003e0.35\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c5\"\u003e\u003cp\u003ePLZT/BNKT\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c6\"\u003e\u003cp\u003eRFE\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c7\"\u003e\u003cp\u003eSol-Gel\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003eJie Zhang et al[\u003cspan citationid=\"CR41\" class=\"CitationRef\"\u003e41\u003c/span\u003e]\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c2\"\u003e\u003cp\u003e21.11\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c3\"\u003e\u003cp\u003e63.3\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c4\"\u003e\u003cp\u003e1.373\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c5\"\u003e\u003cp\u003ePZT/PZO\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c6\"\u003e\u003cp\u003eFE/AFE\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c7\"\u003e\u003cp\u003eSol-Gel\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003eFei Yang et al[\u003cspan citationid=\"CR37\" class=\"CitationRef\"\u003e37\u003c/span\u003e]\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c2\"\u003e\u003cp\u003e32.4\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c3\"\u003e\u003cp\u003e66.9\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c4\"\u003e\u003cp\u003e2.745\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c5\"\u003e\u003cp\u003ePZT/PZO\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c6\"\u003e\u003cp\u003eFE/AFE\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c7\"\u003e\u003cp\u003eSol-Gel\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" 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colname=\"c2\"\u003e\u003cp\u003e16.6\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c3\"\u003e\u003cp\u003e50.4\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c4\"\u003e\u003cp\u003e0.7841\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c5\"\u003e\u003cp\u003ePZO/LNO\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c6\"\u003e\u003cp\u003eAFE\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c7\"\u003e\u003cp\u003eSol-Gel\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003eM. 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G. 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Conclusion","content":"\u003cp\u003e(RFE/AFE)\u003csub\u003en\u003c/sub\u003e PLZT multilayer thin films with various stacking patterns were prepared by the sol-gel/spin-coating method. The effect of stacking orders and AFE layer thicknesses on the energy storage performances were systematically discussed based on the experimental results. An energy storage density of 26.28 J cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e was obtained in (RA)\u003csub\u003e2\u003c/sub\u003e multilayer thin films, which was attributed to the increase in breakdown strength due to the positive interfacial effect. Moreover, the (RA)\u003csub\u003e2\u003c/sub\u003e multilayer thin film exhibits good thermal stability up to 170\u0026deg;C, good frequency stability up to 2kHz, and excellent fatigue endurance after 10\u003csup\u003e6\u003c/sup\u003e charging-discharging cycles. The study provides useful guidelines for designing PLZT-based multilayer thin film capacitors for pulsed power applications.\u003c/p\u003e"},{"header":"Declarations","content":"\u003cp\u003e\u003ch2\u003eDeclaration of Competing Interest\u003c/h2\u003e\u003cp\u003eThe authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.\u003c/p\u003e\u003cp\u003e\u003cstrong\u003eCompeting Interests\u003c/strong\u003e\u003cp\u003eDeclaration of Competing InterestThe authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.\u003c/p\u003e\u003c/p\u003e\u003ch2\u003eAuthor Contribution\u003c/h2\u003e\u003cp\u003eChang Gao: Investigation, Data curation. Lijuan Huang: Methodology, Conceptualization. Chunlin Zhao: Resources, Supervision. Xiao Wu: Resources, Supervision. Tengfei Lin: Resources, Supervision. Cong Lin: Resources, Supervision. Min Gao: Conceptualization, Writing \u0026ndash; review \u0026amp; editing, Funding acquisition.\u003c/p\u003e\u003ch2\u003eAcknowledgement\u003c/h2\u003e\u003cp\u003eThe authors appreciate the support of the National Natural Science Foundation of China (52102126, 52072075, and 12104093), the Natural Science Foundation of Fujian Province (2022J01087, 2022J015552, 2021J05122 and 2021J05123), and the Open Project of Tianjin Key Laboratory of Optoelectronic Detection Technology and System (2024LODTS101).\u003c/p\u003e\u003ch2\u003eData Availability\u003c/h2\u003e\u003cp\u003eThe data that support the findings of this study are available from the corresponding author upon reasonable request.\u003c/p\u003e"},{"header":"References","content":"\u003col\u003e\u003cli\u003e\u003cspan\u003eH. Palneedi, M. Peddigari et al., High-performance dielectric ceramic films for energy storage capacitors: progress and outlook. Adv. 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Interfaces. \u003cb\u003e14\u003c/b\u003e(25), 28997\u0026ndash;29006 (2022). \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttp://doi.org/10.1021/acsami.2c05455\u003c/span\u003e\u003cspan address=\"10.1021/acsami.2c05455\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e\u003c/ol\u003e"}],"fulltextSource":"","fullText":"","funders":[],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":true,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":false,"hideJournal":true,"highlight":"","institution":"","isAcceptedByJournal":true,"isAuthorSuppliedPdf":false,"isDeskRejected":"","isHiddenFromSearch":false,"isInQc":false,"isInWorkflow":false,"isPdf":false,"isPdfUpToDate":true,"isWithdrawnOrRetracted":false,"journal":{"display":true,"email":"[email protected]","identity":"researchsquare","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":true,"externalIdentity":"","sideBox":"","snPcode":"","submissionUrl":"/submission","title":"Research Square","twitterHandle":"researchsquare","acdcEnabled":true,"dfaEnabled":false,"editorialSystem":"","reportingPortfolio":"","inReviewEnabled":false,"inReviewRevisionsEnabled":true},"keywords":"Multilayer thin film, antiferroelectrics, relaxor ferroelectrics, energy storage, PLZT","lastPublishedDoi":"10.21203/rs.3.rs-7912657/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-7912657/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"\u003cp\u003eLead-based multilayer thin film capacitors with excellent energy storage performances have great application potential. However, the effect of stacking patterns on the dielectric behaviors has not been well investigated, especially for the multilayer thin films prepared by chemical solution methods. Here, the relaxor ferroelectric (RFE) (Pb\u003csub\u003e0.92\u003c/sub\u003eLa\u003csub\u003e0.08\u003c/sub\u003e)(Zr\u003csub\u003e0.65\u003c/sub\u003eTi\u003csub\u003e0.35\u003c/sub\u003e)O\u003csub\u003e3\u003c/sub\u003e and antiferroelectric (AFE) (Pb\u003csub\u003e0.98\u003c/sub\u003eLa\u003csub\u003e0.02\u003c/sub\u003e)(Zr\u003csub\u003e0.95\u003c/sub\u003eTi\u003csub\u003e0.05\u003c/sub\u003e)O\u003csub\u003e3\u003c/sub\u003e were chosen to construct diverse multilayer thin film capacitors with different RFE/AFE stacking patterns. Based on their crystal structure, dielectric features, and energy storage behaviors, the effect of stacking orders and AFE phase thicknesses on the capacitor performances were discussed from the perspectives of the positive and negative interface contribution. A superior recoverable energy density of 26.28 J cm\u003csup\u003e\u0026minus;\u0026thinsp;3\u003c/sup\u003e was achieved at a breakdown strength of 3.19 MV cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, accompanied with thermal stability up to 170\u0026deg;C, frequency stability up to 2 kHz, and fatigue endurance after 10\u003csup\u003e6\u003c/sup\u003e charging-discharging cycles. The experimental results and related discussion will support the research and the industrialization of multilayer thin film capacitors.\u003c/p\u003e","manuscriptTitle":"Stacking pattern effect on the energy storage performance of PLZT-based relaxor- ferroelectric/antiferroelectric multilayer thin film capacitors prepared by sol-gel methods","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2025-11-13 18:02:11","doi":"10.21203/rs.3.rs-7912657/v1","editorialEvents":[{"type":"communityComments","content":0}],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"researchsquare","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":true,"externalIdentity":"","sideBox":"","snPcode":"","submissionUrl":"/submission","title":"Research Square","twitterHandle":"researchsquare","acdcEnabled":true,"dfaEnabled":false,"editorialSystem":"","reportingPortfolio":"","inReviewEnabled":false,"inReviewRevisionsEnabled":true}}],"origin":"","ownerIdentity":"694f147a-79bd-427b-8c82-eb94c5a4e386","owner":[],"postedDate":"November 13th, 2025","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"posted","subjectAreas":[],"tags":[],"updatedAt":"2026-01-26T16:00:17+00:00","versionOfRecord":{"articleIdentity":"rs-7912657","link":"https://doi.org/10.1007/s10854-026-16666-6","journal":{"identity":"journal-of-materials-science-materials-in-electronics","isVorOnly":false,"title":"Journal of Materials Science: Materials in Electronics"},"publishedOn":"2026-01-22 15:57:34","publishedOnDateReadable":"January 22nd, 2026"},"versionCreatedAt":"2025-11-13 18:02:11","video":"","vorDoi":"10.1007/s10854-026-16666-6","vorDoiUrl":"https://doi.org/10.1007/s10854-026-16666-6","workflowStages":[]},"version":"v1","identity":"rs-7912657","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-7912657","identity":"rs-7912657","version":["v1"]},"buildId":"8U1c8b4HqxoKbykW_rLl7","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}