Exploring the Pb1−xSrxHfO3 System and Potential for High Capacitive Energy Storage Density and Efficiency
Abstract
The hafnate perovskites PbHfO 3 (antiferroelectric) and SrHfO 3 (“potential” ferroelectric) are studied as epitaxial thin films on SrTiO 3 (001) substrates with the added opportunity of observing a morphotropic phase boundary (MPB) in the Pb 1−xSrxHfO 3 system. The resulting (240)‐oriented PbHfO 3 (Pba 2) films exhibited antiferroelectric switching with a saturation polarization ≈53 µC cm−2 at 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 SrHfO 3 films exhibited neither ferroelectric behavior nor evidence of a polar P 4 mm phase . Instead, the SrHfO 3 films 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 SrHfO 3 removes the potential for MPB, structural and property evolution of the Pb 1−xSrxHfO 3 (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, Pb 0.5 Sr 0.5 HfO 3 produced the best combination of EB = 5.12 ± 0.5 MV cm−1, Ur = 77 ± 5 J cm−3, and η = 97 ± 2%, well out‐performing PbHfO 3 and other antiferroelectric oxides.
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- Authors
- Acharya, M., Banyas, E., Ramesh, M., Jiang, Y., Fernandez, A., Dasgupta, A., Ling, H., Hanrahan, B., Persson, K., Neaton, J. B., & Martin, L. W.
- Affiliations
- Lawrence Berkeley National Laboratory (US)
- University of California, Berkeley (US)
- DEVCOM Army Research Laboratory (US)
- Corresponding author
- Martin, Lane W.
- ORCID
- Venue
- Advanced Materials
- Publisher
- Wiley
- Published
- 2021-10-15
- Volume
- 34
- Issue
- 1
- Pages
- e2105967-e2105967
- ISSN
- 0935-9648 (ISSN-L)
- 1521-4095
- OpenAlex
- W3204726499
- Semantic Scholar
- 223394b6a3ad2e8522ede1cd307ed598c4e9f55d
- Cited by
- 71
- References
- 72
- Citations by year
- 2026: 9 · 2025: 20 · 2024: 13 · 2023: 18 · 2022: 10 · 2021: 1
- FWCI
- 3.04
- Type
- journal article
- Language
- en
- Open access
- closed
- Licence
- Locations
- Advanced Materials (publishedVersion)
- PubMed (publishedVersion)
- eScholarship (California Digital Library) (submittedVersion)
- OSTI OAI (U.S. Department of Energy Office of Scientific and Technical Information) (submittedVersion)
- Funders
- U.S. Department of Energy
- Office of Science
- Basic Energy Sciences (DE‐AC02‐05CH11231)
- National Science Foundation (DMR‐1708615)
- Army Research Office (W911NF‐21‐1‐0126, W911NF‐21‐1‐0118)
- Topics
- Physical Sciences › Materials Science › Materials Chemistry › Ferroelectric and Piezoelectric Materials
- Physical Sciences › Engineering › Electrical and Electronic Engineering › Ferroelectric and Negative Capacitance Devices
- Physical Sciences › Engineering › Biomedical Engineering › Dielectric materials and actuators
- Keywords
- PbHfO3, SrHfO3, morphotropic phase boundary, ferroelectricity, epitaxial thin films, SrTiO3 substrate, electric breakdown strength, hysteresis loss, capacitive energy storage, dielectric constant
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