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<p>Relaxor ferroelectrics are characterized by dispersion of the temperature-dependent dielectric constant with frequency and enhanced electromechanical coupling. These properties arise from the dynamic polar response of correlated nanodomains that are strongly associated with atomic-scale compositional disorder, which disrupts long-range ferroelectric ordering and enables nanodomain formation. Here, we report relaxor properties originating from spontaneous low temperature phase competition in fully cation-ordered antiferroelectric PbMg<sub>0.5</sub>W<sub>0.5</sub>O<sub>3</sub> epitaxial films, including the identification of a new low-energy polar phase. Unlike prototypical relaxors, the <i>B</i>-site cations in coherently strained PbMg<sub>0.5</sub>W<sub>0.5</sub>O<sub>3</sub> films exhibit long-range rocksalt chemical ordering. Temperature-dependent polarization studies reveal the switching behaviors associated with the phase transitions from paraelectric to antiferroelectric to ferroelectric, and the characteristic dielectric relaxation is ascribed instead to phase competition between the polar and antipolar phases mediated by temperature and substrate clamping. This phase competition breaks long-range dipole correlation and leads to dielectric dispersion and relaxor behavior. These findings demonstrate a new paradigm for designing relaxor material properties through engineered phase competition.</p>

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Relaxor behavior in rocksalt cation-ordered material induced by (anti)ferroelectric phase competition

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年6月23日

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  • Yu Yun,
  • Liyan Wu,
  • Drew Behrendt,
  • Hao Pan,
  • Menglin Zhu,
  • Michael Xu,
  • Anthony J. Ruffino,
  • John Carroll,
  • Irina Baraban,
  • Zishen Tian,
  • Xianfei Xu,
  • Dongfang Chen,
  • Brendan M. Hanrahan,
  • Lane W. Martin,
  • James M. LeBeau,
  • Andrew M. Rappe,
  • Ilya Grinberg,
  • Jonathan E. Spanier

摘要

Relaxor ferroelectrics are characterized by dispersion of the temperature-dependent dielectric constant with frequency and enhanced electromechanical coupling. These properties arise from the dynamic polar response of correlated nanodomains that are strongly associated with atomic-scale compositional disorder, which disrupts long-range ferroelectric ordering and enables nanodomain formation. Here, we report relaxor properties originating from spontaneous low temperature phase competition in fully cation-ordered antiferroelectric PbMg0.5W0.5O3 epitaxial films, including the identification of a new low-energy polar phase. Unlike prototypical relaxors, the B-site cations in coherently strained PbMg0.5W0.5O3 films exhibit long-range rocksalt chemical ordering. Temperature-dependent polarization studies reveal the switching behaviors associated with the phase transitions from paraelectric to antiferroelectric to ferroelectric, and the characteristic dielectric relaxation is ascribed instead to phase competition between the polar and antipolar phases mediated by temperature and substrate clamping. This phase competition breaks long-range dipole correlation and leads to dielectric dispersion and relaxor behavior. These findings demonstrate a new paradigm for designing relaxor material properties through engineered phase competition.