Strain-induced lead-free morphotropic phase boundary

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 and Ruijuan Xu ()
Additional contact information
Reza Ghanbari: North Carolina State University
Harikrishnan Kp: Cornell University
Kinnary Patel: University of Arkansas
Hua Zhou: Argonne National Laboratory
Tao Zhou: Argonne National Laboratory
Rui Liu: Argonne National Laboratory
Liyan Wu: Drexel University
Aarushi Khandelwal: Stanford University
Kevin J. Crust: SLAC National Accelerator Laboratory
Sankalpa Hazra: The Pennsylvania State University
John Carroll: Drexel University
Cedric J. G. Meyers: Drexel University
Jiayue Wang: Stanford University
Sergey Prosandeev: University of Arkansas
Huimin Qiao: North Carolina State University
Young-Hoon Kim: Physical Sciences Directorate (PSD), Oak Ridge National Laboratory
Yoji Nabei: North Carolina State University
Miaofang Chi: Physical Sciences Directorate (PSD), Oak Ridge National Laboratory
Dali Sun: North Carolina State University
Nina Balke: North Carolina State University
Martin Holt: Argonne National Laboratory
Venkatraman Gopalan: The Pennsylvania State University
Jonathan E. Spanier: Drexel University
David A. Muller: Cornell University
Laurent Bellaiche: University of Arkansas
Harold Y. Hwang: Stanford University
Ruijuan Xu: North Carolina State University

Nature Communications, 2025, vol. 16, issue 1, 1-11

Abstract: Abstract 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.

Date: 2025
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DOI: 10.1038/s41467-025-63041-w

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