Ultrafast decoupling of polarization and strain in ferroelectric BaTiO3

Le Phuong Hoang, David Pesquera, Gerard N. Hinsley, Robert Carley, Laurent Mercadier, Martin Teichmann, Elena Martina Unterleutner, Daniel Knez, Martina Dienstleder, Saptam Ganguly, Teguh Citra Asmara, Giacomo Merzoni, Sergii Parchenko, Justine Schlappa, Zhong Yin, José Manuel Caicedo Roque, José Santiso, Irena Spasojevic, Cammille Carinan, Tien-Lin Lee, Kai Rossnagel, Jörg Zegenhagen, Gustau Catalan, Ivan A. Vartanyants, Andreas Scherz and Giuseppe Mercurio ()
Additional contact information
Le Phuong Hoang: European XFEL
David Pesquera: Catalan Institute of Nanoscience and Nanotechnology (ICN2), CSIC and BIST, Campus UAB
Gerard N. Hinsley: Photon Science, Deutsches Elektronen-Synchrotron DESY
Robert Carley: European XFEL
Laurent Mercadier: European XFEL
Martin Teichmann: European XFEL
Elena Martina Unterleutner: Graz University of Technology
Daniel Knez: Graz University of Technology
Martina Dienstleder: Graz Centre for Electron Microscopy (ZFE)
Saptam Ganguly: Catalan Institute of Nanoscience and Nanotechnology (ICN2), CSIC and BIST, Campus UAB
Teguh Citra Asmara: European XFEL
Giacomo Merzoni: European XFEL
Sergii Parchenko: European XFEL
Justine Schlappa: European XFEL
Zhong Yin: European XFEL
José Manuel Caicedo Roque: Catalan Institute of Nanoscience and Nanotechnology (ICN2), CSIC and BIST, Campus UAB
José Santiso: Catalan Institute of Nanoscience and Nanotechnology (ICN2), CSIC and BIST, Campus UAB
Irena Spasojevic: Universitat Autònoma de Barcelona
Cammille Carinan: European XFEL
Tien-Lin Lee: Diamond Light Source Ltd.
Kai Rossnagel: Kiel University
Jörg Zegenhagen: Diamond Light Source Ltd.
Gustau Catalan: Catalan Institute of Nanoscience and Nanotechnology (ICN2), CSIC and BIST, Campus UAB
Ivan A. Vartanyants: Photon Science, Deutsches Elektronen-Synchrotron DESY
Andreas Scherz: European XFEL
Giuseppe Mercurio: European XFEL

Nature Communications, 2025, vol. 16, issue 1, 1-10

Abstract: Abstract A fundamental understanding of the interplay between lattice structure, polarization and electrons is pivotal to the optical control of ferroelectrics. The interaction between light and matter enables the remote and wireless control of the ferroelectric polarization on the picosecond timescale, while inducing strain, i.e., lattice deformation. At equilibrium, the ferroelectric polarization is proportional to the strain, and is typically assumed to be so also out of equilibrium. Decoupling the polarization from the strain would remove the constraint of sample design and provide an effective knob to manipulate the polarization by light. Here, upon above-bandgap laser excitation of the prototypical ferroelectric BaTiO3, we induce and measure an ultrafast decoupling between polarization and strain that begins within 350 fs, by softening Ti-O bonds via charge transfer, and lasts for several tens of picoseconds. We show that the ferroelectric polarization out of equilibrium is mainly determined by photoexcited electrons, instead of the strain.

Date: 2025
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DOI: 10.1038/s41467-025-63045-6

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