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Abstract Highly responsive, voltage‐tunable dielectrics are essential for microwave‐telecommunication electronics. Ferroelectric/relaxor materials have been leading candidates for such functionality and have exhibited agile dielectric responses. Here, it is demonstrated that relaxor materials developed from antiferroelectrics can achieve both ultrahigh dielectric response and tunability. The system, based on alloying the archetypal antiferroelectric PbZrO3with the dielectric BaZrO3, exhibits a more complex phase evolution than that in traditional relaxors and is characterized by an unconventional multi‐phase competition between antiferroelectric, ferroelectric, and paraelectric order. This interplay of phases can greatly enhance the local heterogeneities and results in relaxor characteristics while preserving considerable polarizability. Upon studying Pb1‐xBaxZrO3forx= 0‐0.45, Pb0.65Ba0.35ZrO3is found to provide for exceptional dielectric tunability under low bias fields (≈81% at 200 kV cm−1and ≈91% at 500 kV cm−1) at 10 kHz, outcompeting most traditional relaxor ferroelectric films. This high tunability is sustained in the radio‐frequency range, resulting in a high commutation quality factor (>2000 at 1 GHz). This work highlights the phase evolution from antiferroelectrics (with lower, “positive” dielectric tunability) to relaxors (with higher, “negative” tunability), underscoring a promising approach to develop relaxors with enhanced functional capabilities and new possibilities.
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Exploring the Pb 1− x Sr x HfO 3 System and Potential for High Capacitive Energy Storage Density and Efficiency
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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- Award ID(s):
- 1708615
- PAR ID:
- 10361827
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Materials
- Volume:
- 34
- Issue:
- 1
- ISSN:
- 0935-9648
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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