Abstract The hafnate perovskites PbHfO3(antiferroelectric) and SrHfO3(“potential” ferroelectric) are studied as epitaxial thin films on SrTiO3(001) substrates with the added opportunity of observing a morphotropic phase boundary (MPB) in the Pb1−xSrxHfO3system. The resulting (240)‐oriented PbHfO3(Pba2) films exhibited antiferroelectric switching with a saturation polarization ≈53 µC cm−2at 1.6 MV cm−1, weak‐field dielectric constant ≈186 at 298 K, and an antiferroelectric‐to‐paraelectric phase transition at ≈518 K. (002)‐oriented SrHfO3films exhibited neither ferroelectric behavior nor evidence of a polarP4mmphase . Instead, the SrHfO3films exhibited a weak‐field dielectric constant ≈25 at 298 K and no signs of a structural transition to a polar phase as a function of temperature (77–623 K) and electric field (–3 to 3 MV cm−1). While the lack of ferroelectric order in SrHfO3removes the potential for MPB, structural and property evolution of the Pb1−xSrxHfO3(0 ≤x < 1) system is explored. Strontium alloying increased the electric‐breakdown strength (EB) and decreased hysteresis loss, thus enhancing the capacitive energy storage density (Ur) and efficiency (η). The composition, Pb0.5Sr0.5HfO3produced the best combination ofEB = 5.12 ± 0.5 MV cm−1,Ur = 77 ± 5 J cm−3, and η = 97 ± 2%, well out‐performing PbHfO3and other antiferroelectric oxides. 
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                            Giant Energy Density via Mechanically Tailored Relaxor Ferroelectric Behavior of PZT Thick Film
                        
                    
    
            Abstract Relaxor ferroelectrics (RFEs) are being actively investigated for energy‐storage applications due to their large electric‐field‐induced polarization with slim hysteresis and fast energy charging–discharging capability. Here, a novel nanograin engineering approach based upon high kinetic energy deposition is reported, for mechanically inducing the RFE behavior in a normal ferroelectric Pb(Zr0.52Ti0.48)O3(PZT), which results in simultaneous enhancement in the dielectric breakdown strength (EDBS) and polarization. Mechanically transformed relaxor thick films with 4 µm thickness exhibit an exceptionalEDBSof 540 MV m−1and reduced hysteresis with large unsaturated polarization (103.6 µC cm−2), resulting in a record high energy‐storage density of 124.1 J cm−3and a power density of 64.5 MW cm−3. This fundamental advancement is correlated with the generalized nanostructure design that comprises nanocrystalline phases embedded within the amorphous matrix. Microstructure‐tailored ferroelectric behavior overcomes the limitations imposed by traditional compositional design methods and provides a feasible pathway for realization of high‐performance energy‐storage materials. 
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                            - Award ID(s):
- 2133373
- PAR ID:
- 10460721
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Materials
- Volume:
- 35
- Issue:
- 45
- ISSN:
- 0935-9648
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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