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Exploring the Pb 1− x Sr x HfO 3 System and Potential for High Capacitive Energy Storage Density and Efficiency

Journal Article · · Advanced Materials
 [1];  [2];  [3];  [3];  [3];  [3];  [3];  [4];  [5];  [6];  [1]
  1. Department of Materials Science and Engineering University of California, Berkeley Berkeley CA 94720 USA, Materials Sciences Division Lawrence Berkeley National Laboratory Berkeley CA 94720 USA
  2. Materials Sciences Division Lawrence Berkeley National Laboratory Berkeley CA 94720 USA
  3. Department of Materials Science and Engineering University of California, Berkeley Berkeley CA 94720 USA
  4. U.S. Army Research Laboratory Adelphi MD 20783 USA
  5. Department of Materials Science and Engineering University of California, Berkeley Berkeley CA 94720 USA, Materials Sciences Division Lawrence Berkeley National Laboratory Berkeley CA 94720 USA, Molecular Foundry Lawrence Berkeley National Laboratory Berkeley CA 94720 USA
  6. Materials Sciences Division Lawrence Berkeley National Laboratory Berkeley CA 94720 USA, Molecular Foundry Lawrence Berkeley National Laboratory Berkeley CA 94720 USA, Department of Physics University of California, Berkeley Berkeley CA 94720 USA, Kavli Energy Nanosciences Institute University of California Berkeley CA 94720 USA
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− x Sr x HfO 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− x Sr x HfO 3 (0 ≤ x  < 1) system is explored. Strontium alloying increased the electric‐breakdown strength ( E B ) and decreased hysteresis loss, thus enhancing the capacitive energy storage density ( U r ) and efficiency (η). The composition, Pb 0.5 Sr 0.5 HfO 3 produced the best combination of E B  = 5.12 ± 0.5 MV cm −1 , U r  = 77 ± 5 J cm −3 , and η = 97 ± 2%, well out‐performing PbHfO 3 and other antiferroelectric oxides.

Sponsoring Organization:
USDOE
Grant/Contract Number:
AC02-05CH11231
OSTI ID:
1826630
Journal Information:
Advanced Materials, Journal Name: Advanced Materials Journal Issue: 1 Vol. 34; ISSN 0935-9648
Publisher:
Wiley Blackwell (John Wiley & Sons)Copyright Statement
Country of Publication:
Germany
Language:
English

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