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1. Enhanced Piezoelectric, Ferroelectric, and Electrostrictive Properties of Lead‐Free (1‐ x )BCZT‐( x )BCST Electroceramics with Energy Harvesting Capability

   https://doi.org/10.1002/smll.202300549  

   Baraskar, Bharat G. ; Kolekar, Yesappa D. ; Thombare, Balu. R. ; James, Ajit. R. ; Kambale, Rahul C. ; Ramana, C. V. ( May 2023 , Small)

   Next‐generation electronics and energy technologies can now be developed as a result of the design, discovery, and development of novel, environmental friendly lead (Pb)‐free ferroelectric materials with improved characteristics and performance. However, there have only been a few reports of such complex materials’ design with multi‐phase interfacial chemistry, which can facilitate enhanced properties and performance. In this context, herein, novel lead‐free piezoelectric materials (1‐x)Ba_0.95Ca_0.05Ti_0.95Zr_0.05O₃‐(x)Ba_0.95Ca_0.05Ti_0.95Sn_0.05O₃, are reported, which are represented as (1‐x)BCZT‐(x)BCST, with demonstrated excellent properties and energy harvesting performance. The (1‐x)BCZT‐(x)BCST materials are synthesized by high‐temperature solid‐state ceramic reaction method by varyingxin the full range (x= 0.00–1.00). In‐depth exploration research is performed on the structural, dielectric, ferroelectric, and electro‐mechanical properties of (1‐x)BCZT‐(x)BCST ceramics. The formation of perovskite structure for all ceramics without the presence of any impurity phases is confirmed by X‐ray diffraction (XRD) analyses, which also reveals that the Ca²⁺, Zr⁴⁺, and Sn⁴⁺are well dispersed within the BaTiO₃lattice. For all (1‐x)BCZT‐(x)BCST ceramics, thorough investigation of phase formation and phase‐stability using XRD, Rietveld refinement, Raman spectroscopy, high‐resolution transmission electron microscopy (HRTEM), and temperature‐dependent dielectric measurements provide conclusive evidence for the coexistence of orthorhombic + tetragonal (Amm2+P4mm) phases at room temperature. The steady transition ofAmm2crystal symmetry toP4mmcrystal symmetry with increasingxcontent is also demonstrated by Rietveld refinement data and related analyses. The phase transition temperatures, rhombohedral‐orthorhombic (T_R‐O), orthorhombic‐ tetragonal (T_O‐T), and tetragonal‐cubic (T_C), gradually shift toward lower temperature with increasingxcontent. For (1‐x)BCZT‐(x)BCST ceramics, significantly improved dielectric and ferroelectric properties are observed, including relatively high dielectric constantε_r≈ 1900–3300 (near room temperature),ε_r≈ 8800–12 900 (near Curie temperature), dielectric loss, tanδ≈ 0.01–0.02, remanent polarizationP_r≈ 9.4–14 µC cm⁻², coercive electric fieldE_c≈ 2.5–3.6 kV cm⁻¹. Further, high electric field‐induced strainS≈ 0.12–0.175%, piezoelectric charge coefficientd₃₃≈ 296–360 pC N⁻¹, converse piezoelectric coefficient ≈ 240–340 pm V⁻¹, planar electromechanical coupling coefficientk_p≈ 0.34–0.45, and electrostrictive coefficient (Q₃₃)_avg≈ 0.026–0.038 m⁴C⁻²are attained. Output performance with respect to mechanical energy demonstrates that the (0.6)BCZT‐(0.4)BCST composition (x= 0.4) displays better efficiency for generating electrical energy and, thus, the synthesized lead‐free piezoelectric (1‐x)BCZT‐(x)BCST samples are suitable for energy harvesting applications. The results and analyses point to the outcome that the (1‐x)BCZT‐(x)BCST ceramics as a potentially strong contender within the family of Pb‐free piezoelectric materials for future electronics and energy harvesting device technologies.

    

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2. Tunable Magnetic and Optical Anisotropy in ZrO 2 ‐Co Vertically Aligned Nanocomposites

   https://doi.org/10.1002/admi.202300150  

   Zhang, Yizhi ; Song, Jiawei ; Lu, Ping ; Deitz, Julia ; Zhang, Di ; Dou, Hongyi ; Shen, Jianan ; Hu, Zedong ; Zhang, Xinghang ; Wang, Haiyan ( May 2023 , Advanced Materials Interfaces)

   Metamaterials have gained great research interest in recent years owing to their potential for property tunability, multifunctionality, and property coupling. As a new group of self‐assembled thin films, vertically aligned nanocomposite (VAN)‐based hybrid metamaterials have been demonstrated with significant anisotropic physical properties and a broad range of property tailorability, such as optical anisotropy, magnetic anisotropy, hyperbolic dispersion, and enhanced second harmonic generation properties. Herein, self‐assembled ZrO₂‐Co nanocomposite films, with high epitaxial quality and ultra‐fine vertically aligned Co nanopillars (with an average diameter of ≈2 nm) embedded in a ZrO₂matrix, are fabricated using a pulsed laser deposition (PLD) method. The Co pillar density can be effectively tuned by varying the Co concentration in the target, which results in tunable optical properties and magnetic properties. Specifically, a high saturation magnetization of 100 emu cm⁻³, strong out‐of‐plane magnetic anisotropy and tailorable magnetization properties are achieved via tuning the Co nanopillar density. Coupled with hyperbolic dispersion of dielectric constant from 950 to 1500 nm in wavelength, plasmonic Co metal nanopillars, and the unique dielectric ZrO₂matrix, this new nanoscale hybrid metamaterial shows great potential for future integrated optical and magnetic device designs.

    

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3. Relaxor Behavior in Ordered Lead Magnesium Niobate (PbMg 1/3 Nb 2/3 O 3 ) Thin Films

   https://doi.org/10.1002/adfm.201804258  

   Shetty, Smitha ; Damodaran, Anoop ; Wang, Ke ; Yuan, Yakun ; Gopalan, Venkat ; Martin, Lane ; Trolier‐McKinstry, Susan ( November 2018 , Advanced Functional Materials)

   The local compositional heterogeneity associated with the short‐range ordering of Mg and Nb in PbMg_1/3Nb_2/3O₃(PMN) is correlated with its characteristic relaxor ferroelectric behavior. Fully ordered PMN is not prepared as a bulk material. This work examines the relaxor behavior in PMN thin films grown at temperatures below 1073 K by artificially reducing the degree of disorder via synthesis of heterostructures with alternate layers of Pb(Mg_2/3Nb_1/3)O₃and PbNbO₃, as suggested by the random‐site model. 100 nm thick, phase‐pure films are grown epitaxially on (111) SrTiO₃substrates using alternate target timed pulsed‐laser deposition of Pb(Mg_2/3Nb_1/3)O₃and PbNbO₃targets with 20% excess Pb. Selected area electron diffraction confirms the emergence of (1/2, 1/2, 1/2) superlattice spots with randomly distributed ordered domains as large as ≈150 nm. These heterostructures exhibit a dielectric constant of 800, loss tangents of ≈0.03 and 2× remanent polarization of ≈11 µC cm⁻²at room temperature. Polarization–electric field hysteresis loops, Rayleigh data, and optical second‐harmonic generation measurements are consistent with the development of ferroelectric domains below 140 K. Temperature‐dependent permittivity measurements demonstrate reduced frequency dispersion compared to short range ordered PMN films. This work suggests a continuum between normal and relaxor ferroelectric behavior in the engineered PMN thin films.

    

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4. Thermal stability of antiferroelectric-like Al:HfO 2 thin films with TiN or Pt electrodes

   https://doi.org/10.1063/5.0083656  

   Payne, Alexis ; Alex Hsain, H. ; Lee, Younghwan ; Strnad, Nicholas A. ; Jones, Jacob L. ; Hanrahan, Brendan ( June 2022 , Applied Physics Letters)

   HfO 2 -based antiferroelectric-like thin films are increasingly being considered for commercial devices. However, even with initial promise, the temperature sensitivity of electrical properties such as loss tangent and leakage current remains unreported. 50 nm thick, 4 at. % Al-doped HfO 2 thin films were synthesized via atomic layer deposition with both top and bottom electrodes being TiN or Pt. A study of their capacitance vs temperature showed that the Pt/Al:HfO 2 /Pt had a relative dielectric permittivity of 23.30 ± 0.06 at room temperature with a temperature coefficient of capacitance (TCC) of 78 ± 86 ppm/°C, while the TiN/Al:HfO 2 /TiN had a relative dielectric permittivity of 32.28 ± 0.14 at room temperature with a TCC of 322 ± 41 ppm/°C. The capacitance of both devices varied less than 6% over 1 to 1000 kHz from −125 to 125 °C. Both capacitors maintained loss tangents under 0.03 and leakage current densities of 10 −9 –10 −7 A/cm 2 between −125 and 125 °C. The TiN/Al:HfO 2 /TiN capacitor maintained an energy storage density (ESD) of 18.17 ± 0.79 J/cm 3 at an efficiency of 51.79% ± 2.75% over the −125 to 125 °C range. The Pt/Al:HfO 2 /Pt capacitor also maintained a stable ESD of 9.83 ± 0.26 J/cm 3 with an efficiency of 62.87% ± 3.00% over the same temperature range. Such low losses in both capacitors along with their thermal stability make antiferroelectric-like, Al-doped HfO 2 thin films a promising material for temperature-stable microelectronics. 

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5. ZrNb(CO) RF Superconducting Thin Film with High Critical Temperature in the Theoretical Limit

   https://doi.org/10.1002/aelm.202300151  

   Sun, Zeming ; Oseroff, Thomas ; Baraissov, Zhaslan ; Dare, Darrah K. ; Howard, Katrina ; Francis, Benjamin ; Hire, Ajinkya C. ; Sitaraman, Nathan ; Arias, Tomas A. ; Transtrum, Mark K. ; et al ( June 2023 , Advanced Electronic Materials)

   Superconducting radio‐frequency (SRF) resonators are critical components for particle accelerator applications, such as free‐electron lasers, and for emerging technologies in quantum computing. Developing advanced materials and their deposition processes to produce RF superconductors that yield nΩ surface resistances is a key metric for the wider adoption of SRF technology. Here, ZrNb(CO) RF superconducting films with high critical temperatures (T_c) achieved for the first time under ambient pressure are reported. The attainment of aT_cnear the theoretical limit for this material without applied pressure is promising for its use in practical applications. A range ofT_c, likely arising from Zr doping variation, may allow a tunable superconducting coherence length that lowers the sensitivity to material defects when an ultra‐low surface resistance is required. The ZrNb(CO) films are synthesized using a low‐temperature (100 – 200 °C) electrochemical recipe combined with thermal annealing. The phase transformation as a function of annealing temperature and time is optimized by the evaporated Zr‐Nb diffusion couples. Through phase control, one avoids hexagonal Zr phases that are equilibrium‐stable but degradeT_c. X‐ray and electron diffraction combined with photoelectron spectroscopy reveal a system containing cubic β‐ZrNb mixed with rocksalt NbC and low‐dielectric‐loss ZrO₂. Proof‐of‐concept RF performance of ZrNb(CO) on an SRF sample test system is demonstrated. BCS resistance trends lower than reference Nb, while quench fields occur at approximately 35 mT. The results demonstrate the potential of ZrNb(CO) thin films for particle accelerators and other SRF applications.

    

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