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<p>Enhanced susceptibilities in ferroelectrics often arise near phase boundaries between competing ground states. While chemically-induced phase boundaries have enabled ultrahigh electrical and electromechanical responses in lead-based ferroelectrics, precise chemical tuning in lead-free alternatives, such as (K,Na)NbO<sub>3</sub> thin films, remains challenging due to the high volatility of alkali metals. Here, we demonstrate strain-induced morphotropic phase boundary-like polymorphic nanodomain structures in chemically simple, lead-free, epitaxial NaNbO<sub>3</sub> thin films. Combining ab initio simulations, thin-film epitaxy, scanning probe microscopy, synchrotron X-ray diffraction, and electron ptychography, we reveal a labyrinthine structure comprising coexisting monoclinic and bridging triclinic phases near a strain-induced phase boundary. The coexistence of energetically competing phases facilitates field-driven polarization rotation and phase transitions, giving rise to a multi-state polarization switching pathway and large enhancements in dielectric susceptibility and tunability across a broad frequency range. Our results open new possibilities for engineering lead-free thin films with enhanced functionalities for next-generation applications.</p>

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Strain-induced lead-free morphotropic phase boundary

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2025年8月20日

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  • Reza Ghanbari,
  • Harikrishnan KP,
  • Kinnary Patel,
  • Hua Zhou,
  • Tao Zhou,
  • Rui Liu,
  • Liyan Wu,
  • Aarushi Khandelwal,
  • Kevin J. Crust,
  • Sankalpa Hazra,
  • John Carroll,
  • Cedric J. G. Meyers,
  • Jiayue Wang,
  • Sergey Prosandeev,
  • Huimin Qiao,
  • Young-Hoon Kim,
  • Yoji Nabei,
  • Miaofang Chi,
  • Dali Sun,
  • Nina Balke,
  • Martin Holt,
  • Venkatraman Gopalan,
  • Jonathan E. Spanier,
  • David A. Muller,
  • Laurent Bellaiche,
  • Harold Y. Hwang,
  • Ruijuan Xu

摘要

Enhanced susceptibilities in ferroelectrics often arise near phase boundaries between competing ground states. While chemically-induced phase boundaries have enabled ultrahigh electrical and electromechanical responses in lead-based ferroelectrics, precise chemical tuning in lead-free alternatives, such as (K,Na)NbO3 thin films, remains challenging due to the high volatility of alkali metals. Here, we demonstrate strain-induced morphotropic phase boundary-like polymorphic nanodomain structures in chemically simple, lead-free, epitaxial NaNbO3 thin films. Combining ab initio simulations, thin-film epitaxy, scanning probe microscopy, synchrotron X-ray diffraction, and electron ptychography, we reveal a labyrinthine structure comprising coexisting monoclinic and bridging triclinic phases near a strain-induced phase boundary. The coexistence of energetically competing phases facilitates field-driven polarization rotation and phase transitions, giving rise to a multi-state polarization switching pathway and large enhancements in dielectric susceptibility and tunability across a broad frequency range. Our results open new possibilities for engineering lead-free thin films with enhanced functionalities for next-generation applications.