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Synergetic role of strain relaxation and photoexcitation for enhanced nanoscale piezoelectricity in freestanding BaTiO3 thin films

Subhajit Pal1,*, Haoying Sun2,3, Lan-Tien Hsu4, Emanuele Palladino1, Yuefeng Nie2,3, Samuel John5, S. S. Prabhu5, Anna Grünebohm4, and Joe Briscoe1,†

  • 1School of Engineering and Materials Science, Queen Mary University of London, London E14NS, United Kingdom
  • 2National Laboratory of Solid-State Microstructures, Jiangsu Key Laboratory of Artificial Functional Materials, College of Engineering and Applied Sciences, Nanjing University, Nanjing 210093, People's Republic of China
  • 3Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing 210093, People's Republic of China
  • 4Interdisciplinary Center for Advanced Materials Simulation (ICAMS), Center for Interface-Dominated High Performance Materials (ZGH), and Faculty for Physics and Astronomy, Ruhr-University Bochum, 44801 Bochum, Germany
  • 5Department of Condensed Matter Physics and Materials Science, Tata Institute of Fundamental Research, Mumbai 400005, India

  • *Contact author: subhajit.pal@qmul.ac.uk
  • †Contact author: j.briscoe@qmul.ac.uk
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Phys. Rev. Materials 10, 104402 – Published 1 October, 2026

DOI: https://doi.org/10.1103/bp3p-8wrn

Abstract

Strain engineering has emerged as a strategic approach for modulating the piezoelectric and ferroelectric properties of thin films. We investigated local piezoelectric properties in clamped and freestanding epitaxial BaTiO3 films via piezoresponse force microscopy. The freestanding membrane exhibits a ∼300% increase in the effective piezoelectric coefficient compared to the clamped films, driven by increased nonlinearity. Quantitative analysis reveals about fourfold increase in the nonlinearity parameter, originating from enhanced domain wall motion enabled by strain relaxation after removal of substrate-induced clamping. Our molecular dynamics simulations further support about threefold increase in domain-wall velocity in the freestanding film. Additionally, under optical excitation, the membrane exhibits a photoinduced enhancement of the piezoelectric response arising from coupled photostriction effect and light-driven domain wall motion. Density functional theory calculations reveal ∼2% decrease in the out-of-plane lattice parameter of the freestanding membrane under optical excitation, consistent with the observed photoinduced deformation. However, the corresponding change in the clamped film ceases to exist. These results identify substrate clamping as a critical limitation to piezoelectric performance and establish freestanding ferroelectric membranes as promising platforms for low-power electromechanical and optoelectronic devices.

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Phys. Rev. Materials 10, 104402– Published 1 October, 2026
  • Received 17 June 2026
  • Accepted 9 September 2026
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Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.

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