Piezoelectric materials enable the conversion of mechanical energy into electrical energy and vice‐versa. Ultrahigh piezoelectricity has been only observed in single crystals. Realization of piezoelectric ceramics with longitudinal piezoelectric constant (
- Award ID(s):
- 1709025
- NSF-PAR ID:
- 10300935
- Date Published:
- Journal Name:
- Research
- Volume:
- 2021
- ISSN:
- 2639-5274
- Page Range / eLocation ID:
- 1 to 7
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Abstract d 33) close to 2000 pC N–1, which combines single crystal‐like high properties and ceramic‐like cost effectiveness, large‐scale manufacturing, and machinability will be a milestone in advancement of piezoelectric ceramic materials. Here, guided by phenomenological models and phase‐field simulations that provide conditions for flattening the energy landscape of polarization, a synergistic design strategy is demonstrated that exploits compositionally driven local structural heterogeneity and microstructural grain orientation/texturing to provide record piezoelectricity in ceramics. This strategy is demonstrated on [001]PC‐textured and Eu3+‐doped Pb(Mg1/3Nb2/3)O3‐PbTiO3(PMN‐PT) ceramics that exhibit the highest piezoelectric coefficient (small‐signald 33of up to 1950 pC N–1and large‐signald 33* of ≈2100 pm V–1) among all the reported piezoelectric ceramics. Extensive characterization conducted using high‐resolution microscopy and diffraction techniques in conjunction with the computational models reveals the underlying mechanisms governing the piezoelectric performance. Further, the impact of losses on the electromechanical coupling is identified, which plays major role in suppressing the percentage of piezoelectricity enhancement, and the fundamental understanding of loss in this study sheds light on further enhancement of piezoelectricity. These results on cost‐effective and record performance piezoelectric ceramics will launch a new generation of piezoelectric applications. -
Abstract 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 )Ba0.95Ca0.05Ti0.95Zr0.05O3‐(x )Ba0.95Ca0.05Ti0.95Sn0.05O3, 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 varyingx in 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 ofAmm2 crystal symmetry toP4mm crystal symmetry with increasingx content is also demonstrated by Rietveld refinement data and related analyses. The phase transition temperatures, rhombohedral‐orthorhombic (TR‐O), orthorhombic‐ tetragonal (TO‐T), and tetragonal‐cubic (TC), gradually shift toward lower temperature with increasingx content. 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 coefficientd 33≈ 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 (Q 33)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. -
Abstract Many technologically critical materials are metastable under ambient conditions, yet the understanding of how to rationally design and guide the synthesis of these materials is limited. This work presents an integrated approach that targets a metastable lead‐free piezoelectric polymorph of SrHfO3. First‐principles calculations predict that the previous experimentally unrealized, metastable P4
mm phase of SrHfO3should exhibit a direct piezoelectric response (d33) of 36.9 pC N−1(compared tod 33= 0 for the ground state). Combining computationally optimized substrate selection and synthesis conditions lead to the epitaxial stabilization of the polar P4mm phase of SrHfO3on SrTiO3. The films are structurally consistent with the theory predictions. A ferroelectric‐induced large signal effective converse piezoelectric response of 5.2 pm V−1for a 35 nm film is observed, indicating the ability to predict and target multifunctionality. This illustrates a coupled theory‐experimental approach to the discovery and realization of new multifunctional polymorphs. -
Abstract Piezoresponse force microscopy (PFM) is widely used for characterization and exploration of the nanoscale properties of ferroelectrics. However, quantification of the PFM signal is challenging due to the convolution of various extrinsic and intrinsic contributions. Although quantification of the PFM amplitude signal has received considerable attention, quantification of the PFM phase signal has not been addressed. A properly calibrated PFM phase signal can provide valuable information on the sign of the local piezoelectric coefficient—an important and nontrivial issue for emerging ferroelectrics. In this work, two complementary methodologies to calibrate the PFM phase signal are discussed. The first approach is based on using a standard reference sample with well‐known independently measured piezoelectric coefficients, while the second approach exploits the electrostatic sample–cantilever interactions to determine the parasitic phase offset. Application of these methodologies to studies of the piezoelectric behavior in ferroelectric HfO2‐based thin‐film capacitors reveals intriguing variations in the sign of the longitudinal piezoelectric coefficient,
d 33,eff. It is shown that the piezoelectric properties of the HfO2‐based capacitors are inherently sensitive to their thickness, electrodes, as well as deposition methods, and can exhibit wide variations including ad 33,effsign change within a single device. -
Additive manufacturing (AM), also known as three-dimensional (3D) printing, is thriving as an effective and robust method in fabricating architected piezoelectric structures, yet most of the commonly adopted printing techniques often face the inherent speed-accuracy trade-off, limiting their speed in manufacturing sophisticated parts containing micro-/nanoscale features. Herein, stabilized, photo-curable resins comprising chemically functionalized piezoelectric nanoparticles (PiezoNPs) were formulated, from which microscale architected 3D piezoelectric structures were printed continuously via micro continuous liquid interface production ( μ CLIP) at speeds of up to ~60 μ m s -1 , which are more than 10 times faster than the previously reported stereolithography-based works. The 3D-printed functionalized barium titanate (f-BTO) composites reveal a bulk piezoelectric charge constant d 33 of 27.70 pC N -1 with the 30 wt% f-BTO. Moreover, rationally designed lattice structures that manifested enhanced, tailorable piezoelectric sensing performance as well as mechanical flexibility were tested and explored in diverse flexible and wearable self-powered sensing applications, e.g., motion recognition and respiratory monitoring.more » « less